Oxime compounds and the use thereof

ABSTRACT

The invention relates to oxime compounds of Formula (I) and pharmaceutically acceptable salts, prodrugs, or solvates thereof, wherein X is hydrogen, optionally substituted aryl, optionally substituted heteroaryl or the like; Y is CO, SO 2 , CR 3 R 4  or the like; Z is optionally substituted lower alkyl, optionally substituted aryl or the like; W is optionally substituted lower alkylene or optionally substituted lower alkenylene, R 3  and R 4  are each independently hydrogen, lower alkyl or the like; p is 0, 1, or 2 and q is 0, 1 or 2. The invention is also directed to the use compounds of Formula I to treat, prevent or ameliorate a disorder responsive to the blockade of calcium channels, and particularly N-type calcium channels. Compounds of the present invention are especially useful for treating pain.

BACKGROUND OF THE INVENTION

1. Field of the Invention

This invention is in the field of medicinal chemistry. The inventionrelates to oxime compounds and the discovery that these compounds act asblockers of calcium (Ca²⁺) channels.

2. Background Art

Calcium ions play fundamental roles in the regulation of many cellularprocesses. It is therefore essential that their intracellular levels bemaintained under strict, yet dynamic control (Davila, H. M., Annals ofthe New York Academy of Sciences, pp. 102-117 (1999)). Voltage-gatedcalcium channels (VGCC) serve as one of the important mechanisms forfast calcium influx into the cell. Calcium channels arehetero-oligomeric proteins consisting of a pore-forming subunit (α1),which is able to form functional channels on its own in heterologousexpression systems, and a set of auxiliary or regulatory subunits.Calcium channels have been classified based on their pharmacologicaland/or electrophysiological properties. The classification ofvoltage-gated calcium channels divides them into three groups: (i) highvoltage-activated (HVA) channels, which include L-, N-, P-, and Q-types;(ii) intermediate (IVA) voltage-activated R-type channels; and (iii) lowvoltage-activated (LVA) T-type channels (Davila, supra). Voltage-gatedcalcium channels (VGCC) are also known as voltage-dependent calciumchannels (VDCC) or voltage-sensitive calcium channels (VSCC).

Voltage-sensitive calcium channels (VSCC) regulate intracellular calciumconcentration, which affects various important neuronal functions suchas cellular excitability, neurotransmitter release, hormone secretion,intracellular metabolism, neurosecretory activity and gene expression(Hu et al., Bioorganic & Medicinal Chemistry 8:1203-1212 (2000)). N-typechannels are found mainly in central and peripheral neurons, beingprimarily located on presynaptic nerve terminals. These channelsregulate the calcium flux required for depolarization-evoked release ofa transmitter from synaptic endings. The transmission of pain signalsfrom the periphery to the central nervous system (CNS) is mediated byN-type calcium channels located in the spinal cord (Song et al., J. Med.Chem. 43:3474-3477 (2000)).

The six types of calcium channels (i.e., L, N, P, Q, R, and T) areexpressed throughout the nervous system (Wallace, M. S., The ClinicalJournal of Pain 16:580-585 (2000)). Voltage-sensitive calcium channelsof the N-type exist in the superficial laminae of the dorsal horn andare thought to modulate nociceptive processing by a central mechanism.Blockade of the N-type calcium channel in the superficial dorsal hornmodulates membrane excitability and inhibits neurotransmitter release,resulting in pain relief. Wallace (supra) suggests that based on animalmodels, N-type calcium channel antagonists have a greater analgesicpotency than sodium channel antagonists. N-type calcium channel blockershave usefulness for neuroprotection and analgesia. Ziconotide, which isa selective N-type calcium channel blocker, has been found to haveanalgesic activity in animal models and neuroprotective activity infocal and global ischemia models (Song et al., supra). Examples of knowncalcium channel blockers include flunarizine, fluspirilene, cilnipide,PD 157767, SB-201823, SB-206284, NNC09-0026, and PD 151307 (Hu et al.,supra).

Blockade of N-type channels can prevent and/or attenuate subjective painas well as primary and/or secondary hyperalgesia and allodynia in avariety of experimental and clinical conditions (Vanegas, H. et al.,Pain 85:9-18 (2000)). N-type voltage-gated calcium channels (VGCC) playa major role in the release of synaptic mediators such as glutamate,acetylcholine, dopamine, norepinephrine, gamma-aminobutyric acid (GABA)and calcitonin gene-related peptide (CGRP).

Inhibition of voltage-gated L-type calcium channels has been shown to bebeneficial for neuroprotection (Song et al., supra). However, inhibitionof cardiac L-type calcium channels can lead to hypotension. It isbelieved that a rapid and profound lowering of arterial pressure tendsto counteract the neuroprotective effects of L-type calcium channelblockers. A need exists for antagonists that are selective for N-typecalcium channels over L-type calcium channels to avoid potentialhypotensive effects. Similar compounds to those of the present inventionare described in WO2004/083 167, WO99/24399, JP50-084523, U.S. Pat. No.3,577,441, WO 2005048933, U.S. Pat. No. 5,880,138, GB 2231048 and thelike, but the structures of these compounds are different from those ofthe present invention.

BRIEF SUMMARY OF THE INVENTION

The present invention is related to the use of oxime compoundsrepresented by Formula I, I′, I″, II or II′, below, and thepharmaceutically acceptable salts, prodrugs and solvates thereof, asblockers of calcium (Ca²⁺) channels. Certain compounds of Formula I, I′,I″, II or II′ show selectivity as N-type calcium channel blockers. Theinvention is also related to treating, preventing or ameliorating adisorder responsive to the blockade of calcium channels in a mammalsuffering from excess activity of said channels by administering aneffective amount of a compound of Formula I, I′, I″, II or II′, or apharmaceutically acceptable salt, prodrug or solvate thereof, asdescribed herein. Specifically, the invention is related to treating,preventing or ameliorating a disorder responsive to the blockade ofN-type calcium channels in a mammal suffering from excess activity ofsaid channels by administering an effective amount of a compound ofFormula I, I′, I″, II or II′, or a pharmaceutically acceptable salt,prodrug or solvate thereof, as described herein.

One aspect of the present invention is directed to novel compounds ofFormula I or II, or a pharmaceutically acceptable salt, prodrug orsolvate thereof.

Another aspect of the present invention is directed to the use of thenovel compounds of Formula T. I″ or II or compounds of Formula I′ orII′, or a pharmaceutically acceptable salt, prodrug or solvate thereof,as blockers of N-type calcium channels. A further aspect of the presentinvention is to provide a method for treating, preventing orameliorating stroke, neuronal damage resulting from head trauma,epilepsy, pain (e.g., acute pain, chronic pain, which includes but isnot limited to, neuropathic pain and inflammatory pain, or surgicalpain), migraine, a mood disorder, schizophrenia, a neurodegenerativedisorder (e.g., Alzheimer's disease, amyotrophic lateral sclerosis(ALS), or Parkinson's disease), depression, anxiety, a psychosis,hypertension, or cardiac arrhythmia, by administering an effectiveamount of a compound of Formula I, I′, I″, II or II′, or apharmaceutically acceptable salt, prodrug or solvate thereof, to amammal in need of such treatment, prevention or amelioration.

A further aspect of the present invention is to provide a pharmaceuticalcomposition useful for treating, preventing or ameliorating a disorderresponsive to the blockade of calcium ion channels, especially N-typecalcium ion channels, said pharmaceutical composition containing aneffective amount of a compound of Formula I, I′, I″, II or II′, or apharmaceutically acceptable salt, prodrug or solvate thereof, in amixture with one or more pharmaceutically acceptable carriers.

Also, an aspect of the invention is to provide a method of modulatingcalcium channels, especially N-type calcium channels, in a mammal,wherein said method comprises administering to the mammal an effectiveamount of at least one compound of Formula I, I′, I″, II or II′, or apharmaceutically acceptable salt, prodrug or solvate thereof.

A further aspect of the present invention is to provide radiolabeledcompounds of Formula I, I′, I″, II or II′ and the use of such compounds,or their pharmaceutically acceptable salts, prodrugs or solvates, asradioligands for their binding site on the calcium channel.

A further aspect of the invention is to provide a method for screening acandidate compound for the ability to bind to a receptor using a ³H, ¹¹Cor ¹⁴C radiolabeled compound of Formula I, I′, I″, II or II′, or apharmaceutically acceptable salt, prodrug or solvate thereof. Thismethod comprises a) introducing a fixed concentration of theradiolabeled compound to the receptor to form a mixture; b) titratingthe mixture with a candidate compound; and c) determining the binding ofthe candidate compound to said receptor.

A further aspect of the invention is to provide the use of a compound ofFormula I, I′, I″, II or II′, or a pharmaceutically acceptable salt,prodrug or solvate thereof, in the manufacture of a medicament fortreating, preventing or ameliorating stroke, neuronal damage resultingfrom head trauma, epilepsy, pain, migraine, a mood disorder,schizophrenia, a neurodegenerative disorder, depression, anxiety, apsychosis, hypertension, or cardiac arrhythmia in a mammal. In apreferred embodiment, the invention provides the use of a compound ofFormula I, I′, I″, II or II′, or a pharmaceutically acceptable salt,prodrug or solvate thereof, in the manufacture of a medicament fortreating, preventing or ameliorating acute pain, chronic pain, orsurgical pain.

Additional embodiments and advantages of the invention will be set forthin part in the description that follows, and will flow from thedescription, or may be learned by practice of the invention. Theembodiments and advantages of the invention will be realized andattained by means of the elements and combinations particularly pointedout in the appended claims.

It is to be understood that both the foregoing summary and the followingdetailed description are exemplary and explanatory only and are notrestrictive of the invention, as claimed.

DETAILED DESCRIPTION OF THE INVENTION

One aspect of the present invention is based upon the use of compoundsof Formula I, I′, I″, II or II′, and the pharmaceutically acceptablesalts, prodrugs and solvates thereof, as blockers of Ca²⁺ channels. Inview of this property, compounds of Formula I, I′, I″, II or II′, andthe pharmaceutically acceptable salts, prodrugs and solvates thereof,are useful for treating disorders responsive to the blockade of calciumion channels. In one aspect, compounds of Formula I, I′, I″, II or II′,and the pharmaceutically acceptable salts, prodrugs and solvatesthereof, selectively block N-type calcium ion channels and, thus, areuseful for treating disorders responsive to the selective blockade ofN-type calcium ion channels.

The present invention provides

1) A compound having the Formula I:

a pharmaceutically acceptable salt, a prodrug or a solvate thereof,wherein:

-   -   W is absent, optionally substituted lower alkylene or optionally        substituted lower alkenylene,    -   X is optionally substituted aryl, optionally substituted        heterocyclyl, optionally substituted cycloalkyl or optionally        substituted cycloalkenyl and    -   When W is optionally substituted lower alkylene or optionally        substituted lower alkenylene, then X can additionally be        hydrogen;    -   Y is CO, SO_(m) or CR³R⁴;

Z is optionally substituted lower alkyl, optionally substituted loweralkenyl, optionally substituted lower alkynyl, optionally substitutedlower alkoxy, optionally substituted lower alkenyloxy, optionallysubstituted lower alkynyloxy, optionally substituted amino, optionallysubstituted lower alkylthio, optionally substituted lower alkenylthio,optionally substituted lower alkynylthio, optionally substitutedcycloalkyl, optionally substituted cycloalkenyl, optionally substitutedaryl or optionally substituted heterocyclyl,

when Y is CO, then Z can additionally be optionally substituted acyl,optionally substituted carbamoyl, optionally substituted cycloalkyloxy,optionally substituted cycloalkenyloxy, optionally substituted aryloxyor optionally substituted heterocyclyloxy,

when Y is CR³R⁴, then Z can additionally be hydrogen, hydroxy, halogen,carboxy, optionally substituted lower alkoxycarbonyl, optionallysubstituted lower alkylthio, optionally substituted acyl, optionallysubstituted acyloxy, optionally substituted lower alkylsulfonyl,optionally substituted lower alkylsulfonyloxy, optionally substitutedlower alkylsulfinyl, optionally substituted carbamoyl, optionallysubstituted carbamoyloxy, optionally substituted sulfamoyl, optionallysubstituted sulfamoyloxy, optionally substituted aryloxy, optionallysubstituted aryloxycarbonyl, optionally substituted arylthio, optionallysubstituted arylsulfonyl, optionally substituted arylsulfinyl,optionally substituted arylsulfonyloxy, optionally substitutedarylsulfinyloxy, optionally substituted heterocyclyloxy, optionallysubstituted heterocyclyloxycarbonyl, optionally substitutedheterocyclylthio, optionally substituted heterocyclylsulfonyl,optionally substituted heterocyclylsulfinyl, optionally substitutedheterocyclylsulfonyloxy, optionally substituted heterocyclylsulfinyloxy,

-   -   R³ and T⁴ are each independently hydrogen, halogen, lower alkyl,        halo(lower)alkyl, hydroxy(lower)alkyl, amino, lower alkylamino,        optionally substituted cycloalkyl, optionally substituted        cycloalkenyl, optionally substituted aryl or optionally        substituted heterocyclyl, or together with the carbon atom to        which they are attached form optionally substituted carbocycle        or optionally substituted heterocycle;    -   R is lower alkyl, hydroxy(lower)alkyl, lower alkoxy(lower)alkyl,        carboxy, lower alkoxycarbonyl, carbamoyl or lower        alkylcarbamoyl,    -   m is 1 or 2,    -   p is 0, 1 or2, and    -   q is 0, 1 or 2 with the following provisos:

i) when Y is SO₂, then Z is not lower alkyl substituted with at leastone substituent selected from CONHOH, COOH and lower alkoxycarbonyl,

ii) Y-Z is not benzoyl, acetyl, carbamoyl or lower alkoxycarbonyl,

iii) when Y is CO, then Z is not methylene substituted withheterocyclidene, and

iv) when Y is SO₂, then —W—X is not 2-tetrahydrofuryl.

1′) A compound having the Formula II:

and pharmaceutically acceptable salts, prodrugs and solvates thereof,wherein:

-   -   X is optionally substituted aryl, optionally substituted        heterocyclyl, optionally substituted cycloalkyl or optionally        substituted cycloalkenyl;    -   Y is CO, SO_(m), or CR³R⁴;    -   Z is optionally substituted lower alkyl, optionally substituted        lower alkenyl, optionally substituted lower alkynyl, optionally        substituted lower alkoxy, optionally substituted lower        alkenyloxy, optionally substituted lower alkynyloxy, optionally        substituted amino, optionally substituted lower alkylthio,        optionally substituted lower alkenylthio, optionally substituted        lower alkynylthio, optionally substituted cycloalkyl, optionally        substituted cycloalkenyl, optionally substituted aryl or        optionally substituted heterocyclyl,

when Y is CO, then Z can additionally be optionally substituted acyl oroptionally substituted carbamoyl,

when Y is CR³R⁴, then Z can additionally be hydrogen, hydroxy, halogen,optionally substituted lower alkoxy, carboxy, optionally substitutedlower alkoxycarbonyl, optionally substituted lower alkylthio, optionallysubstituted acyl, optionally substituted acyloxy, optionally substitutedlower alkylsulfonyl, optionally substituted lower alkylsulfonyloxy,optionally substituted lower alkylsulfinyl, optionally substitutedcarbamoyl, optionally substituted carbamoyloxy, optionally substitutedsulfamoyl, optionally substituted sulfamoyloxy,

optionally substituted aryloxy, optionally substituted aryloxycarbonyl,optionally substituted arylthio, optionally substituted arylsulfonyl,optionally substituted arylsulfinyl, optionally substitutedarylsulfonyloxy, optionally substituted arylsulfinyloxy, optionallysubstituted heterocyclyloxy, optionally substitutedheterocyclyloxycarbonyl, optionally substituted heterocyclylthio,optionally substituted heterocyclylsulfonyl, optionally substitutedheterocyclylsulfinyl, optionally substituted heterocyclylsulfonyloxy,optionally substituted heterocyclylsulfinyloxy,

-   -   R¹ and R² are each independently hydrogen, halogen, lower alkyl,        halo(lower)alkyl, optionally substituted cycloalkyl, optionally        substituted cycloalkenyl, optionally substituted aryl or        optionally substituted heterocyclyl;    -   R³ and R⁴ are each independently hydrogen, halogen, lower alkyl,        halo(lower)alkyl, hydroxy(lower)alkyl, amino, lower alkylamino,        optionally substituted cycloalkyl, optionally substituted        cycloalkenyl, optionally substituted aryl or optionally        substituted heterocyclyl;    -   R is lower alkyl, hydroxy(lower)alkyl, lower alkoxy(lower)alkyl,        carboxy, lower alkoxycarbonyl, carbamoyl or lower        alkylcarbamoyl,    -   n is 0, 1, 2 or 3 and    -   m is 1 or 2,    -   p is 0, 1 or 2, with the following provisos:

i) when Y is SO₂, then Z is not lower alkyl substituted with at leastone substituent selected from CONHOH, COOH and lower alkoxycarbonyl,

ii) Y-Z is not benzoyl, acetyl, carbamoyl or lower alkoxycarbonyl,

iii) when Y is CO, then Z is not methylene substituted withheterocyclidene, and

iv) when Y is SO₂, then X is not tetrahydrofuran.

2) The compounds of the above 1), wherein q is 1.

3) The compound of the above 1) or 2), wherein W is (CR¹R²)n, n is 0, 1,2 or 3, R¹ and R² are each independently hydrogen, halogen, lower alkyl,halo(lower)alkyl, hydroxy(lower)alkyl, lower alkoxy(lower)alkyl,optionally substituted aryl(lower)alkyl, optionally substitutedaryloxy(lower)alkyl, optionally substituted heterocyclyl(lower)alkyl,optionally substituted

heterocyclyloxy(lower)alkyl, optionally substituted cycloalkyl,optionally substituted cycloalkenyl, optionally substituted aryl oroptionally substituted heterocyclyl and X is optionally substitutedaryl, optionally substituted heterocyclyl, optionally substitutedcycloalkyl or optionally substituted cycloalkenyl.

4) The compound of any of the above 1), 1′), 2) or 3), wherein W isoptionally substituted methylene.

5) The compound of any of the above 1),1′) or 2) to 4), wherein X isoptionally substituted phenyl or optionally substituted pyridyl.

6) The compound of any one of the above 1), 1′) or 2) to 5), wherein Yis CO or SO₂.

7) The compound of any one of the above 1), 1′) or 2) to 6), wherein Zis optionally substituted lower alkyl or optionally substituted phenyl.

8) A pharmaceutical composition, comprising the compound of any of theabove 1), 1′) or 2) to 7) and a pharmaceutically acceptable carrier.

9) A method of treating, preventing or ameliorating a disorderresponsive to the blockade of calcium channels in a mammal sufferingfrom said disorder, comprising administering to a mammal in need of suchtreatment, prevention or amelioration an effective amount of a compoundof any of the above 1), 1′) or 2) to 7).

10) The method of the above 9), wherein a disorder responsive to theblockade of N-type calcium channels is treated, prevented orameliorated.

11) A method for treating, preventing or ameliorating stroke,neuronaldamage resulting from head trauma, epilepsy, pain, migraine, a mooddisorder, schizophrenia, a neurodegenerative disorder, depression,anxiety, a psychosis, hypertension or cardiac arrhythmia in a mammal,comprising administering an effective amount of a compound of any of theabove 1), 1′) or 2) to 7).

12) The method of the above 11), wherein the method is for treating,preventing or ameliorating pain selected from chronic pain, acute pain,and surgical pain.

13) A method of modulating calcium channels in a mammal, comprisingadministering to the mammal at least one compound of any one of theabove 1), 1′) or 2) to 7).

14) The method of the above 13), wherein the N-type calcium channel ismodulated.

15) A compound having the Formula I as described in the above 1), 1′) or2) to 7), wherein the compound is ³H, ¹¹C, or ¹⁴C radiolabeled.

16) A method of screening a candidate compound for the ability to bindto a receptor using a radiolabeled compound of the above 15), comprisinga) introducing a fixed concentration of the radiolabeled compound to thereceptor to form a mixture; b) titrating the mixture with a candidatecompound; and c) determining the binding of the candidate compound tosaid receptor.

17) Use of a compound of Formula I as claimed in any one of the above1), 1′) or 2) to 7) in the manufacture of a medicament for treating,preventing or ameliorating stroke, neuronal damage resulting from headtrauma, epilepsy, pain, migraine, a mood disorder, schizophrenia, aneurodegenerative disorder, depression, anxiety, a psychosis,hypertension or cardiac arrhythmia in a mammal.

18) Use of a compound of Formula I as claimed in any one of the above1), 1′) or 2) to 7) in the manufacture of a medicament for treating,preventing or ameliorating pain selected from chronic pain, acute pain,and surgical pain.

19) A pharmaceutical composition for modulating calcium channels in amammal, comprising the compound having the Formula I′:

a pharmaceutically acceptable salt, a prodrug or a solvate thereof,wherein:

-   -   W is absent, optionally substituted lower alkylene or optionally        substituted lower alkenylene,    -   X is optionally substituted aryl, optionally substituted        heterocyclyl, optionally substituted cycloalkyl or optionally        substituted cycloalkenyl and    -   When W is optionally substituted lower alkylene or optionally        substituted lower alkenylene, then X can additionally be        hydrogen;    -   Y is CO, SO_(m) or CR³R⁴;    -   Z is optionally substituted lower alkyl, optionally substituted        lower alkenyl, optionally substituted lower alkynyl, optionally        substituted lower alkoxy, optionally substituted lower        alkenyloxy, optionally substituted lower alkynyloxy, optionally        substituted amino, optionally substituted lower alkylthio,        optionally substituted lower alkenylthio, optionally substituted        lower alkynylthio, optionally substituted cycloalkyl, optionally        substituted cycloalkenyl, optionally substituted aryl or        optionally substituted heterocyclyl,    -   when Y is CO, then Z can additionally be optionally substituted        acyl, optionally substituted carbamoyl, optionally substituted        cycloalkyloxy, optionally substituted cycloalkenyloxy,        optionally substituted aryloxy or optionally substituted        heterocyclyloxy,    -   when Y is CR³R⁴, then Z can additionally be hydrogen, hydroxy,        halogen, carboxy, optionally substituted lower alkoxycarbonyl,        optionally substituted lower alkylthio, optionally substituted        acyl, optionally substituted acyloxy, optionally substituted        lower alkylsulfonyl, optionally substituted lower        alkylsulfonyloxy, optionally substituted lower alkylsulfinyl,        optionally substituted carbamoyl, optionally substituted        carbamoyloxy, optionally substituted sulfamoyl, optionally        substituted sulfamoyloxy,    -   optionally substituted aryloxy, optionally substituted        aryloxycarbonyl, optionally substituted arylthio, optionally        substituted arylsulfonyl, optionally substituted arylsulfinyl,        optionally substituted arylsulfonyloxy, optionally substituted        arylsulfinyloxy, optionally substituted heterocyclyloxy,        optionally substituted heterocyclyloxycarbonyl, optionally        substituted heterocyclylthio, optionally substituted        heterocyclylsulfonyl, optionally substituted        heterocyclylsulfinyl, optionally substituted        heterocyclylsulfonyloxy, optionally substituted        heterocyclylsulfinyloxy,    -   when Z is optionally substituted cycloalkyl, optionally        substituted cycloalkenyl, optionally substituted aryl or        optionally substituted heterocyclyl, then Y can additionally be        absent;

R³ and R⁴ are each independently hydrogen, halogen, lower alkyl,halo(lower)alkyl, hydroxy(lower)alkyl, amino, lower alkylamino,optionally substituted cycloalkyl, optionally substituted cycloalkenyl,optionally substituted aryl or optionally substituted heterocyclyl, ortogether with the carbon atom to which they are attached form optionallysubstituted carbocycle or optionally substituted heterocycle;

-   -   R is lower alkyl, hydroxy(lower)alkyl, lower alkoxy(lower)alkyl,        carboxy, lower alkoxycarbonyl, carbamoyl or lower        alkylcarbamoyl,    -   m is 1 or 2,    -   p is 0, 1 or 2, and    -   q is 0, 1 or 2

and a pharmaceutically acceptable carrier.

19′) A pharmaceutical composition for modulating calcium channels in amammal, comprising the compound having the Formula II′:

and pharmaceutically acceptable salts, prodrugs and solvates thereof,wherein:

-   -   X is optionally substituted aryl, optionally substituted        heterocyclyl, optionally substituted cycloalkyl or optionally        substituted cycloalkenyl;    -   Y is CO, SO_(m) or CR³R⁴;    -   Z is optionally substituted lower alkyl, optionally substituted        lower alkenyl, optionally substituted lower alkynyl, optionally        substituted lower alkoxy, optionally substituted lower        alkenyloxy,optionally substituted lower alkynyloxy, optionally        substituted amino, optionally substituted lower alkylthio,        optionally substituted lower alkenylthio, optionally substituted        lower alkynylthio, optionally substituted cycloalkyl, optionally        substituted cycloalkenyl, optionally substituted aryl or        optionally substituted heterocyclyl,    -   when Y is CO, then Z can additionally be optionally substituted        acyl or optionally substituted carbamoyl,    -   when Y is CR³R⁴, then Z can additionally be hydrogen, hydroxy,        halogen, carboxy, optionally substituted lower alkoxycarbonyl,        optionally substituted lower alkylthio, optionally substituted        acyl, optionally substituted acyloxy, optionally substituted        lower alkylsulfonyl, optionally substituted lower        alkylsulfonyloxy, optionally substituted lower alkylsulfinyl,        optionally substituted carbamoyl, optionally substituted        carbamoyloxy, optionally substituted sulfamoyl, optionally        substituted sulfamoyloxy, optionally substituted aryloxy,        optionally substituted aryloxycarbonyl, optionally substituted        arylthio, optionally substituted arylsulfonyl, optionally        substituted arylsulfinyl, optionally substituted        arylsulfonyloxy, optionally substituted arylsulfinyloxy,        optionally substituted heterocyclyloxy, optionally substituted        heterocyclyloxycarbonyl, optionally substituted        heterocyclylthio, optionally substituted heterocyclylsulfonyl,        optionally substituted heterocyclylsulfinyl, optionally        substituted heterocyclylsulfonyloxy, optionally substituted        heterocyclylsulfinyloxy, when Z is optionally substituted        cycloalkyl, optionally substituted cycloalkenyl, optionally        substituted aryl or optionally substituted heterocyclyl, then Y        can additionally be absent;    -   R¹ and R² are each independently hydrogen, halogen, lower alkyl,        halo(lower)alkyl, optionally substituted cycloalkyl, optionally        substituted cycloalkenyl, optionally substituted aryl or        optionally substituted heterocyclyl;    -   R³ and R⁴ are each independently hydrogen, halogen, lower alkyl,        halo(lower)alkyl, hydroxy(lower)alkyl, amino, lower alkylamino,        optionally substituted cycloalkyl, optionally substituted        cycloalkenyl, optionally substituted aryl or optionally        substituted heterocyclyl;    -   R is lower alkyl, hydroxy(lower)alkyl, lower alkoxy(lower)alkyl,        carboxy, lower alkoxycarbonyl, carbamoyl or lower        alkylcarbamoyl,    -   n is 0, 1, 2 or 3 and    -   m is 1 or 2,    -   p is 0, 1 or 2

and a pharmaceutically acceptable carrier.

20) The pharmaceutical composition of the above 19) or 19′), wherein qis 1.

21) The pharmaceutical composition of the above 19),19′) or 20), whereinW is (CR¹R²)n, n is 0, 1, 2 or 3, R¹ and R² are each independentlyhydrogen, halogen, lower alkyl, halo(lower)alkyl, hydroxy(lower)alkyl,lower alkoxy(lower)alkyl, optionally substituted aryl(lower)alkyl,optionally substituted aryloxy(lower)alkyl, optionally substitutedheterocyclyl(lower)alkyl, optionally substitutedheterocyclyloxy(lower)alkyl, optionally substituted cycloalkyl,optionally substituted cycloalkenyl, optionally substituted aryl oroptionally substituted heterocyclyl and X is optionally substitutedaryl, optionally substituted heterocyclyl, optionally substitutedcycloalkyl or optionally substituted cycloalkenyl.

22) A method of treating, preventing or ameliorating a disorderresponsive to the blockade of calcium channels in a mammal sufferingfrom said disorder, comprising administering to a mammal in need of suchtreatment, prevention or amelioration an effective amount of a compoundhaving the Formula I′ described in the above 19).

23) A method for treating, preventing or ameliorating stroke, neuronaldamage resulting from head trauma, epilepsy, pain, migraine, a mooddisorder, schizophrenia, a neurodegenerative disorder, depression,anxiety, a psychosis, hypertension or cardiac arrhythmia in a mammal,comprising administering an effective amount of a compound having theFormula I′ described in the above 19).

24) The method of the above 23), wherein the method is for treating,preventing or ameliorating pain selected from chronic pain, acute pain,and surgical pain.

25) A method of modulating calcium channels in a mammal, comprisingadministering to the mammal at least one compound having the Formula I′described in the above 19).

26) A method of screening a candidate compound for the ability to bindto a receptor using a ³H, ¹¹C, or ¹⁴C radiolabeled compound having theFormula I′ described in the above 19), comprising a) introducing a fixedconcentration of the radiolabeled compound to the receptor to form amixture; b) titrating the mixture with a candidate compound; and c)determining the binding of the candidate compound to said receptor.

27) Use of a compound having the Formula I′ described in the above 19)in the manufacture of a medicament for the treating, preventing orameliorating stroke, neuronal damage resulting from head trauma,epilepsy, pain, migraine, a mood disorder, schizophrenia, aneurodegenerative disorder, depression, anxiety, a psychosis,hypertension or cardiac arrhythmia in a mammal.

28) Use of a compound having the Formula I′ described in the above 19)in the manufacture of a medicament for the treating, preventing orameliorating pain selected from chronic pain, acute pain, and surgicalpain.

In the present specification, the term “halogen” includes fluorine,chlorine, bromine and iodine. Fluorine or chlorine is preferable. Thehalogen parts of “halo(lower)alkyl”, “halocycloalkyl”,“halocycloalkenyl”, “haloheterocyclyl”, “haloacyl” and “haloaryl” arethe same as the above “halogen”.

The term “lower alkyl” includes straight or branched chain alkyl having1 to 10 carbon atoms, preferably 1 to 6 carbon atoms and most preferably1 to 3 carbon atoms. For example, included are methyl, ethyl, n-propyl,isopropyl, n-butyl, isobutyl, sec-butyl, tert-butyl, n-pentyl,isopentyl, neopentyl, hexyl, isohexyl, n-heptyl, isoheptyl, n-octyl,isooctyl, n-nonyl, n-decyl and the like.

The optional substituents in “optionally substituted lower alkyl”,include

1) halogen,

2) hydroxy,

3)carboxy,

4) mercapto,

5) cyano,

6) nitro,

7) lower alkoxy optionally substituted with at least one substituentselected from the group consisting of Group A and Group C,

8) acyl optionally substituted with at least one substituent selectedform the group consisting of Group A, Group B and Group C,

9) acyloxy optionally substituted with at least one substituent selectedform the group consisting of Group A, Group B and Group C

10) lower alkoxycarbonyl optionally substituted with at least onesubstituent selected form the group consisting of Group A and Group C,

11) aryloxycarbonyl optionally substituted with at least one substituentselected form the group consisting of Group A, Group B and Group C,

12) lower alkylthio optionally substituted with at least one substituentselected form the group consisting of Group A and Group C,

13) lower alkylsulfonyl optionally substituted with at least onesubstituent selected form the group consisting of Group A and Group C,

14) amino optionally substituted with at least one substituent selectedform the group consisting of Group A, Group B and Group C

15) imino optionally substituted with at least one substituent selectedform the group consisting of Group A, Group B and Group C,

16) carbamoyl optionally substituted with at least one substituentselected form the group consisting of Group A, Group B and Group C,

17) carbamoyloxy optionally substituted with at least one substituentselected form the group consisting of Group A, Group B and Group C,

18) thiocarbamoyl optionally substituted with at least one substituentselected form the group consisting of Group A, Group B and Group C,

19) cycloalkyl optionally substituted with at least one substituentselected form the group consisting of Group A, Group B and Group C,

20) cycloalkenyl optionally substituted with at least one substituentselected form the group consisting of Group A, Group B and Group C,

21) aryl optionally substituted with at least one substituent selectedform the group consisting of Group A, Group B and Group C,

22) heterocyclyl optionally substituted with at least one substituentselected form the group consisting of Group A, Group B, Group C and oxo,

23) aryloxy optionally substituted with at least one substituentselected form the group consisting of Group A, Group B and Group C,

24) arylthio optionally substituted with at least one substituentselected form the group consisting of Group A, Group B and Group C,

25) arylsulfonyl optionally substituted with at least one substituentselected form the group consisting of Group A, Group B and Group C,

26) heterocyclylsulfonyl optionally substituted with at least onesubstituent selected form the group consisting of Group A, Group B,Group C, and oxo

and the like.

Group A includes hydroxy, halogen, cyano, nitro, lower alkoxy,halo(lower)alkoxy, hydroxy(lower)alkoxy, aryl(lower)alkoxy, acyl,haloacyl, aminoacyl, acyloxy, carboxy, lower alkoxycarbonyl, carbamoyl,lower alkylcarbamoyl, and optionally substituted amino, wherein thesubstituents are selected from the group consisting of halogen, hydroxy,lower alkyl,hydroxy(lower)alkyl, lower alkoxy(lower)alkyl, acyl,cycloalkyl, aryl and heterocyclyl.

Group B includes lower alkyl, halo(lower)alkyl, hydroxy(lower)alkyl,lower alkoxy(lower)alkyl, amino(lower)alkyl, loweralkylamino(lower)alkyl, cycloalkyl(lower)alkyl, aryl(lower)alkyl,halogenoaryl(lower)alkyl, hydroxyaryl(lower)alkyl,heterocyclyl(lower)alkyl, halogenoheterocyclyl(lower)alkyl andhydroxyaryl(lower)alkyl.

Group C includes optionally substituted cycloalkyl, optionallysubstituted cycloalkenyl, optionally substituted aryl and optionallysubstituted heterocyclyl, wherein the substituents are selected from thegroup consisting of Group A, Group B and oxo. The term “optionallysubstituted lower alkyl” refers to a lower alkyl that can be substitutedwith one or more of the above-mentioned substituents at any possiblepositions.

The lower alkyl parts of “lower alkoxy”, “lower alkoxycarbonyl”, “loweralkylsulfonyl”, “lower alkylsulfonyloxy”, “lower alkylsulfinyl”, “loweralkylthio”, “halo(lower)alkyl”, “hydroxy(lower)alkyl”,“amino(lower)alkyl”, “lower alkylamino(lower)alkyl”, “aryl(lower)alkyl”,“aryloxy(lower)alkyl”, “halo(lower)alkoxy”, “hydroxy(lower)alkoxy”,“lower alkoxy(lower)alkyl”, “lower alkoxy(lower)alkoxy”,“aryl(lower)alkoxy”, “lower alkylamino”, “hydroxy(lower)alkylamino”,“lower alkylcarbamoyl”, “lower alkylcarbamoyloxy”, “loweralkylslulfamoyl”, “lower alkylsulfamoyloxy”, “heterocyclyl(lower)alkyl”,“heterocyclyloxy(lower)alkyl”, “lower alkylenedioxy” and “loweralkylene” are as defined for “lower alkyl”.

The optional substituents in “optionally substituted lower alkoxy”,“optionally substituted lower alkoxycarbonyl”, “optionally substitutedlower alkylsulfonyl”, “optionally substituted lower alkylsulfonyloxy”,“optionally substituted lower alkylsulfinyl” and “optionally substitutedlower alkylthio” include those defined for “optionally substituted loweralkyl”.

The optional substituents in “optionally substituted lower alkylene”include halogen, lower alkyl, halo(lower)alkyl, hydroxy(lower)alkyl,lower alkoxy(lower)alkyl, optionally substituted aryl(lower)alkyl,optionally substituted aryloxy(lower)alkyl, optionally substitutedheterocyclyl(lower)alkyl, optionally substitutedheterocyclyloxy(lower)alkyl, optionally substituted cycloalkyl,optionally substituted cycloalkenyl, optionally substituted aryl oroptionally substituted heterocyclyl and the like.

The term “lower alkenyl” refers to straight or branched chain alkenyl of2 to 10 carbon atoms, preferably 2 to 8 carbon atoms, more preferably 3to 6 carbon atoms having at least one double bond at any possiblepositions. For example, useful lower alkenyl groups include vinyl,propenyl, isopropenyl, butenyl, isobutenyl, prenyl, butadienyl,pentenyl, isopentenyl, pentadienyl, hexenyl, isohexenyl, hexadienyl,heptenyl, octenyl, nonenyl, decenyl and the like.

The optional substituents in “optionally substituted lower alkenyl”include those defined for “optionally substituted lower alkyl”.

The lower alkenyl parts of “lower alkenyloxy”, “lower alkenylthio” and“lower alkenylene” are the same as the above “lower alkenyl”. Theoptional substituents in “optionally substituted lower alkenyl”,“optionally substituted lower alkenyloxy” and “optionally substitutedlower alkenylthio” include those defined for “optionally substitutedlower alkyl”.

The optional substituents in “optionally substituted lower alkenylene”include halogen, lower alkyl, halo(lower)alkyl, hydroxy(lower)alkyl,lower alkoxy(lower)alkyl, optionally substituted aryl(lower)alkyl,optionally substituted aryloxy(lower)alkyl, optionally substitutedheterocyclyl(lower)alkyl, optionally substitutedheterocyclyloxy(lower)alkyl, optionally substituted cycloalkyl,optionally substituted cycloalkenyl, optionally substituted aryl oroptionally substituted heterocyclyl and X is optionally substitutedaryl, optionally substituted heterocyclyl, optionally substitutedcycloalkyl, optionally substituted cycloalkenyl and the like.

The term “acyl” refers to straight or branched chain aliphatic acylhaving 1 to I 0 carbon atoms, preferably 1 to 6 carbon atoms, morepreferably 1 to 4 carbon atoms, cyclic aliphatic acyl having 4 to 9carbon atoms, preferably 4 to 7 carbon atoms, aroyl andheterocyclylcarbonyl. Suitable acyl groups include, for example, formyl,acetyl, propionyl, butyryl, isobutyryl, valeryl, pivaloyl, hexanoyl,acryloyl, propioloyl, methacryloyl, crotonoyl, cyclopropylcarbonyl,cyclohexylcarbonyl, cyclooctylcarbonyl, benzoyl, pyridinecarbonyl,pyrimidinecarbonyl, piperidincarbonyl, piperazinocarbonyl,morphorinocarbonyl and the like.

The optional substituents in “optionally substituted acyl” include thosedefined for “optionally substituted lower alkyl.”

The optional substituents for aroyl or heterocyclylcarbonyl are

1) lower alkyl optionally substituted with at least one substituent fromGroup B,

2) the same as those defined for “optionally substituted lower alkyl”and the like.

The acyl parts in “acyloxy” “haloacyl” and “aminoacyl” are those definedfor “acyl”.

The optional substituents in “optionally substituted acyloxy” includethose defined for “optionally substituted acyl.”

The term “carbocycle” refers to a carbocycle having 3 to 6 carbon atomsand includes cyclopropyl, cyclobutyl, cyclopentyl, cyclohexyl and thelike.

The term “cycloalkyl” refers to a carbocycle having 3 to 6 carbon atomsand includes cyclopropyl, cyclobutyl, cyclopentyl, cyclohexyl and thelike. Cycloalkyl can be fused with one or more carbocycles.

The cycloalkyl parts in “hydroxycycloalkyl” and “halocycloalkyl” arethose defined for “cycloalkyl”.

The term “cycloalkenyl” refers to a group having at least one doublebond at any possible positions in the above “cycloalkyl”. Cycloalkenylcan be fused with one or more carbocycles and/or aryl. Examples arecyclopropenyl, cyclobutenyl, cyclopentenyl, cyclohexenyl,cyclohexadienyl and fluorenyl.

The optional substituents in “optionally substituted carbocycle”,“optionally substituted cycloalkyl” and “optionally substitutedcycloalkenyl” are

1) lower alkyl optionally substituted with at least one substituentselected from the group consisting of Group A and Group C, and

2) the same as those defined for “optionally substituted lower alkyl”.

The terms “optionally substituted carbocycle”, “optionally substitutedcycloalkyl” and “optionally substituted cycloalkenyl” refers to“carbocycle”, “cycloalkyl” and “cycloalkenyl” defined above that can besubstituted with one or more of these substituents, respectively.

The optional substituents in “optionally substituted amino”, exemplifiedare

1) lower alkyl optionally substituted with at least one substituentselected from the group consisting of Group A and Group C, and

2) the same as those defined for “optionally substituted lower alkyl”.

The term “lower alkylamino” refers to mono-alkylamino and di-alkylamino.

The optional substituents in “optionally substituted carbamoyl” are

1) lower alkyl optionally substituted with at least one substituentselected from the group consisting of Group A and Group C,

2) Group B and

3) Group C.

The optional substituents in “optionally substituted carbamoyloxy” arethose defined for “optionally substituted carbamoyl”.

The optional substituents in “optionally substituted sulfamoyl” or“optionally substituted sulfamoyloxy” are those defined for “optionallysubstituted carbamoyl”.

The term “aryl” includes phenyl, naphthyl, anthryl, phenanthryl, indenyland the like. Phenyl is preferable.

The aryl parts of “aryloxy”, “aryloxycarbonyl”, “arylthio”,“arylsulfonyl”,

“arylsulfinyl”, “arylsulfonyloxy”, “arylsulfinyloxy” “aryl(lower)alkyl”,“aryloxy(lower)alkyl”,“aryl(lower)alkoxy”, “hydroxyaryl” and “haloaryl”are the same as the above “aryl”.

The term “heterocyclyl” or “heterocycle” refers to a heterocyclic groupcontaining at least one heteroatom arbitrarily selected from the groupof O, S and N. Suitable heterocyclyl groups are, for example, 5- or6-membered heteroaryl groups such as pyrrolyl, imidazolyl, pyrazolyl,pyridyl, pyridazinyl, pyrimidinyl, oxazolyl, isoxazolyl, oxadiazolyl,isothiazolyl, thiazolyl, thiadiazolyl, furyl and thienyl; fusedheterocyclyl groups having two rings, such as indolyl, isoindolyl,indazolyl, indolizinyl, indolinyl, isoindolinyl, quinolyl, isoquinolyl,cinnolinyl, phthalazinyl, quinazolinyl, naphthyridinyl, quinoxalinyl,purinyl, pteridinyl, benzopyranyl, benzimidazolyl, benzisoxazolyl,benzoxazolyl benzoxadiazolyl, benzisothiazolyl, benzothiazolyl,benzothiadiazolyl, benzofuryl, isobenzofuryl, benzothienyl,benzotriazolyl, imidazopyridyl, triazoropyridyl, imidazothiazolyl,pyrazinopyridazinyl, quinazolinyl, quinolyl, isoquinolyl,naphthyridinyl, benzomorpholinyl, benzomorpholino, benzodioxolanyl,tetrahydroquinolyl and tetrahydrobenzothienyl; fused heterocyclyl groupshaving three rings such as carbazolyl, acridinyl, xanthenyl,phenothiazinyl, phenoxathiinyl, phenoxazinyl and dibenzofuryl; andnon-aromatic heterocyclyl such as dioxanyl, thiiranyl, oxiranyl,oxathiolanyl, azetidinyl, thianyl, pyrrolidinyl, pyrrolinyl,imidazolidinyl, imidazolinyl, pyrazolidinyl, pyrazolinyl, piperidyl,piperazinyl, morpholinyl, morpholino, thiomorpholinyl, thiomorpholino,dihydropyridyl, dihydroisoxazolyl, tetrahydrofuryl, tetrahydropyranyl,tetrahydrothiazolyl and tetrahydroisothiazolyl.

The heterocyclyl parts of “heterocyclyloxy”, “heterocyclyl(lower)alkyl”,“heterocyclyloxy(lower)alkyl”, “heterocyclyloxycarbonyl”,“heterocyclylthio”, “heterocyclylsulfonyl”, “heterocyclylsulfinyl”,“heterocyclylsulfonyloxy”,“heterocyclylsulfinyloxy”“hydroxyheterocyclyl”, “haloheterocyclyl” and“oxoheterocyclyl” are the same as the above “heterocyclyl”.

The optional substituents in “optionally substituted aryl”, “optionallysubstituted aryloxy”, “optionally substituted aryloxycarbonyl”,“optionally substituted arylthio”, “optionally substituted arylsulfony”,“optionally substituted arylsulfinyl”, “optionally substitutedarylsulfonyloxy”, “optionally substituted arylsulfonyloxy”, “optionallysubstituted aryl(lower)alkyl”, “optionally substitutedaryloxy(lower)alkyl”, “optionally substituted heterocycle”, “optionallysubstituted heterocyclyl”, “optionally substitutedheterocyclyl(lower)alkyl”, “optionally substitutedheterocyclyloxy(lower)alkyl”, “optionally substituted heterocyclyloxy”,“optionally substituted heterocyclyloxycarbonyl”, “optionallysubstituted heterocyclylthio”, “optionally substitutedheterocyclylsulfonyl”, “optionally substituted heterocyclylsulfinyl”,“optionally substituted heterocyclylsulfonyloxy”, “optionallysubstituted heterocyclylsulfinyloxy”, “optionally substituted phenyl”and “optionally substituted pyridyl” are

1) the same as those defined for “optionally substituted lower alkyl”,

2) lower alkyl optionally substituted with at least one substituentselected from the Group A and Group C,

3) oxo and

4) lower alkylenedioxy.

These substituents can attach to one or more of any possible positions.

The term “heterocyclidene” includes a divalent heterocyclyl group whichcan be induced by removing two hydrogens on the same carbon atom.Heterocycle part of the “heterocyclidene” is the same as the above“heterocyclyl”. Examples of “heterocyclidene” istetrahydrobenzazepinylidene and the like.

In the compound of Formula I or I′, Z includes the followings.

1) when Y is CO, then

Z is optionally substituted lower alkyl, optionally substituted loweralkenyl, optionally substituted lower alkynyl, optionally substitutedlower alkoxy, optionally substituted lower alkenyloxy, optionallysubstituted lower alkynyloxy, optionally substituted amino, optionallysubstituted lower alkylthio, optionally substituted lower alkenylthio,optionally substituted lower alkynylthio, optionally substitutedcycloalkyl, optionally substituted cycloalkenyl, optionally substitutedaryl, optionally substituted heterocyclyl, optionally substituted acyl,optionally substituted carbamoyl, optionally substituted cycloalkyloxy,optionally substituted cycloalkenyloxy, optionally substituted aryloxyor optionally substituted heterocyclyloxy,

2) when Y is SOm, then

Z is optionally substituted lower alkyl, optionally substituted loweralkenyl, optionally substituted lower alkynyl, optionally substitutedlower alkoxy, optionally substituted lower alkenyloxy, optionallysubstituted lower alkynyloxy, optionally substituted amino, optionallysubstituted lower alkylthio, optionally substituted lower alkenylthio,optionally substituted lower alkynylthio, optionally substitutedcycloalkyl, optionally substituted cycloalkenyl, optionally substitutedaryl, or optionally substituted heterocyclyl,

3) when Y is CR³R⁴, then

Z is optionally substituted lower alkyl, optionally substituted loweralkenyl, optionally substituted lower alkynyl, optionally substitutedlower alkoxy, optionally substituted lower alkenyloxy, optionallysubstituted lower alkynyloxy, optionally substituted amino, optionallysubstituted lower alkylthio, optionally substituted lower alkenylthio,optionally substituted lower alkynylthio, optionally substitutedcycloalkyl, optionally substituted cycloalkenyl, optionally substitutedaryl, optionally substituted heterocyclyl, hydrogen, hydroxy, halogen,carboxy, optionally substituted lower alkoxycarbonyl, optionallysubstituted lower alkylthio, optionally substituted acyl, optionallysubstituted acyloxy, optionally substituted lower alkylsulfonyl,optionally substituted lower alkylsulfonyloxy, optionally substitutedlower alkylsulfinyl, optionally substituted carbamoyl, optionallysubstituted carbamoyloxy, optionally substituted sulfamoyl, optionallysubstituted sulfamoyloxy, optionally substituted aryloxy, optionallysubstituted aryloxycarbonyl, optionally substituted arylthio, optionallysubstituted arylsulfonyl, optionally substituted arylsulfinyl,optionally substituted arylsulfonyloxy, optionally substitutedarylsulfinyloxy, optionally substituted heterocyclyloxy, optionallysubstituted heterocyclyloxycarbonyl, optionally substitutedheterocyclylthio, optionally substituted heterocyclylsulfonyl,optionally substituted heterocyclylsulfinyl, optionally substitutedheterocyclylsulfonyloxy or optionally substitutedheterocyclylsulfinyloxy.

The compound of the present invention includes the solvate thereof andhydrate is preferable. An example of the solvate is a solvate with anorganic solvent and/or water. The compound of the present invention maycooperate with arbitrary numbers of water molecules to give a hydratethereof.

The phrase “when Y is SO₂, then Z is not lower alkyl substituted with atleast one substituent selected from CONHOH, COOH and loweralkoxycarbonyl” means the exclusion of the compound wherein Y is SO₂ andZ is lower alkyl substituted with CONHOH, COOH and/or loweralkoxycarbonyl. In this case, the lower alkyl of Z can be substitutedwith additional substituents.

Illustrative Oxime Compounds are the compounds of the following formulaI″:

wherein X is one of the followings:

In another embodiment, the compounds of the formula I″ wherein (CR¹R²)nis absent (hereinafter referred to as CR¹R² is Ca), CH₂ (hereinafterreferred to as CR¹R² is Cb), CHMe (hereinafter referred to as CR¹R² isCc), CMe₂ (hereinafter referred to as CR¹R² is Cd), CH₂CH₂ (hereinafterreferred to as CR¹R² is Ce) or CHPh (hereinafter referred to as CR¹R² isCf).

In another embodiment, the compounds of the formula I″ wherein Y-Z isone of the followings:

In another embodiment, the compounds I″ wherein the combination of X,CR¹R² and Y-Z (X, CR¹R², Y-Z) is one of the followings:

(X,CR¹R²,Y-Z)=(Xa,Ca,YZa),(Xa,Ca,YZb),(Xa,Ca,YZc),(Xa,Ca,YZd),(Xa,Ca,YZe),(Xa,Ca,YZf),(Xa,Ca,YZg),(Xa,Ca,YZh),(Xa,Ca,YZi),(Xa,Ca,YZj),(Xa,Ca,YZk),(Xa,Ca,YZl),(Xa,Ca,YZm),(Xa,Ca,YZn),(Xa,Ca,YZo),(Xa,Ca,YZp),(Xa,Ca,YZq),(Xa,Ca,YZr),(Xa,Ca,YZs),(Xa,Ca,YZt),(Xa,Ca,YZu),(Xa,Ca,YZv),(Xa,Ca,YZw),(Xa,Ca,YZx),(Xa,Ca,YZy),(Xa,Ca,YZz),(Xa,Ca,YZaa),(Xa,Ca,YZab),(Xa,Ca,YZac),(Xa,Ca,YZad),(Xa,Ca,YZae),(Xa,Ca,YZaf),(Xa,Ca,YZag),(Xa,Ca,YZah),(Xa,Ca,YZai),(Xa,Ca,YZaj),(Xa,Ca,YZak),(Xa,Ca,YZal),(Xa,Ca,YZam),(Xa,Ca,YZan),(Xa,Ca,YZao),(Xa,Ca,YZap),(Xa,Ca,YZaq),(Xa,Ca,YZar),(Xa,Ca,YZas),(Xa,Ca,YZat),(Xa,Ca,YZau),(Xa,Ca,YZav),(Xa,Ca,YZaw),(Xa,Ca,YZax),(Xa,Ca,YZay),(Xa,Ca,YZaz),(Xa,Ca,YZba),(Xa,Ca,YZbb),(Xa,Ca,YZbc),(Xa,Ca,YZbd),(Xa,Ca,YZbe),(Xa,Ca,YZbf),(Xa,Ca,YZbg),(Xa,Ca,YZbh),(Xa,Ca,YZbi),(Xa,Ca,YZbj),(Xa,Ca,YZbk),(Xa,Ca,YZbl),(Xa,Ca,YZbm),(Xa,Ca,YZbn),(Xa,Ca,YZbo),(Xa,Ca,YZbp),(Xa,Ca,YZbq),(Xa,Ca,YZbr),(Xa,Ca,YZbs),(Xa,Ca,YZbt),(Xa,Ca,YZbu),(Xa,Ca,YZbv),(Xa,Ca,YZbw),(Xa,Ca,YZbx),(Xa,Ca,YZby),(Xa,Ca,YZbz),(Xa,Ca,YZca),(Xa,Ca,YZcb),(Xa,Ca,YZcc),(Xa,Ca,YZcd),(Xa,Ca,YZce),(Xa,Ca,YZcf),(Xa,Ca,YZcg),(Xa,Ca,YZch),(Xa,Ca,YZci),(Xa,Ca,YZcj),(Xa,Ca,YZck),(Xa,Ca,YZcl),(Xa,Ca,YZcm),(Xa,Ca,YZcn),(Xa,Ca,YZco),(Xa,Ca,YZcp),(Xa,Ca,YZcq),(Xa,Ca,YZcr),(Xa,Ca,YZcs),(Xa,Ca,YZct),(Xa,Ca,YZcu),(Xa,Ca,YZcv),(Xa,Ca,YZcw),(Xa,Ca,YZcx),(Xa,Ca,YZcy),(Xa,Ca,YZcz),(Xa,Ca,YZda),(Xa,Ca,YZdb),(Xa,Ca,YZdc),(Xa,Ca,YZdd),(Xa,Ca,YZde),(Xa,Ca,YZdf),(Xa,Ca,YZdg),(Xa,Ca,YZdh),(Xa,Ca,YZdi),(Xa,Ca,YZdj),(Xa,Ca,YZdk),(Xa,Ca,YZdl),(Xa,Ca,YZdm),(Xa,Ca,YZdn),(Xa,Ca,YZdo),(Xa,Ca,YZdp),(Xa,Ca,YZdq),(Xa,Ca,YZdr),(Xa,Ca,YZds),(Xa,Ca,Yzdt),(Xa,Ca,YZdu),(Xa,Ca,YZdv),(Xa,Ca,YZdw),(Xa,Ca,YZdx),(Xa,Ca,YZdy),(Xa,Ca,YZdz),(Xa,Ca,YZea),(Xa,Ca,YZeb),(Xa,Ca,YZec),(Xa,Ca,YZed),(Xa,Ca,YZee),(Xa,Ca,YZef),(Xa,Ca,YZeg),(Xa,Ca,YZeh),(Xa,Ca,YZei),(Xa,Ca,YZej),(Xa,Ca,YZek),(Xa,Ca,YZel),(Xa,Ca,YZem),(Xa,Ca,YZen),(Xa,Ca,YZeo),(Xa,Ca,YZep),(Xa,Ca,YZeq),(Xa,Ca,YZer),(Xa,Ca,YZes),(Xa,Ca,YZet),(Xa,Ca,YZeu),(Xa,Ca,YZev),(Xa,Ca,YZew),(Xa,Ca,YZex),(Xa,Ca,YZey),(Xa,Ca,YZez),(Xa,Ca,YZfa),(Xa,Ca,YZfb),(Xa,Ca,YZfc),(Xa,Ca,YZfd),(Xa,Ca,YZfe),(Xa,Ca,YZff),(Xa,Ca,YZfg),(Xa,Ca,YZfh),(Xa,Ca,YZfi),(Xa,Ca,YZfj),(Xa,Ca,YZfk),(Xa,Ca,YZfl),(Xa,Ca,YZfm),(Xa,Ca,YZfn),(Xa,Ca,YZfo),(Xa,Ca,YZfp),(Xa,Ca,YZfq),(Xa,Ca,YZfr),(Xa,Ca,YZfs),(Xa,Ca,YZft),(Xa,Ca,YZfu),(Xa,Ca,YZfv),(Xa,Ca,YZfw),(Xa,Ca,YZfx),(Xa,Ca,YZfy),(Xa,Ca,YZfz),(Xa,Ca,YZga),(Xa,Ca,YZgb),(Xa,Ca,YZgc),(Xa,Ca,YZgd),(Xa,Ca,YZge),(Xa,Ca,YZgf),(Xa,Ca,YZgg),(Xa,Ca,YZgh),(Xa,Ca,YZgi),(Xa,Ca,YZgj),(Xa,Ca,YZgk),(Xa,Ca,YZgl),(Xa,Ca,YZgm),(Xa,Ca,YZgn),(Xa,Ca,YZgo),(Xa,Ca,YZgp),(Xa,Ca,YZgq),(Xa,Ca,YZgr),(Xa,Ca,YZgs),(Xa,Ca,YZgt),(Xa,Cb,YZa),(Xa,Cb,YZb),(Xa,Cb,YZc),(Xa,Cb,YZd),(Xa,Cb,YZe),(Xa,Cb,YZf),(Xa,Cb,YZg),(Xa,Cb,YZh),(Xa,Cb,YZi),(Xa,Cb,YZj),(Xa,Cb,YZk),(Xa,Cb,YZl),(Xa,Cb,YZm),(Xa,Cb,YZn),(Xa,Cb,YZo),(Xa,Cb,YZp),(Xa,Cb,YZq),(Xa,Cb,YZr),(Xa,Cb,YZs),(Xa,Cb,YZt),(Xa,Cb,YZu),(Xa,Cb,YZv),(Xa,Cb,YZw),(Xa,Cb,YZx),(Xa,Cb,YZy),(Xa,Cb,YZz),(Xa,Cb,YZaa),(Xa,Cb,YZab),(Xa,Cb,YZac),(Xa,Cb,YZad),(Xa,Cb,YZae),(Xa,Cb,YZaf),(Xa,Cb,YZag),(Xa,Cb,YZah),(Xa,Cb,YZai),(Xa,Cb,YZaj),(Xa,Cb,YZak),(Xa,Cb,YZal),(Xa,Cb,YZam);(Xa,Cb,YZan),(Xa,Cb,YZao),(Xa,Cb,YZap),(Xa,Cb,YZaq),(Xa,Cb,YZar),(Xa,Cb,YZas),(Xa,Cb,YZat),(Xa,Cb,YZau),(Xa,Cb,YZav),(Xa,Cb,YZaw),(Xa,Cb,YZax),(Xa,Cb,YZay),(Xa,Cb,YZaz),(Xa,Cb,YZba),(Xa,Cb,YZbb),(Xa,Cb,YZbc),(Xa,Cb,YZbd),(Xa,Cb,YZbe),(Xa,Cb,YZbf),(Xa,Cb,YZbg),(Xa,Cb,YZbh),(Xa,Cb,YZbi),(Xa,Cb,YZbj),(Xa,Cb,YZbk),(Xa,Cb,YZbl),(Xa,Cb,YZbm),(Xa,Cb,YZbn),(Xa,Cb,YZbo),(Xa,Cb,YZbp),(Xa,Cb,YZbq),(Xa,Cb,YZbr),(Xa,Cb,YZbs),(Xa,Cb,YZbt);(Xa,Cb,YZbu),(Xa,Cb,YZbv),(Xa,Cb,YZbw),(Xa,Cb,YZbx),(Xa,Cb,YZby),(Xa,Cb,YZbz),(Xa,Cb,YZca),(Xa,Cb,YZcb),(Xa,Cb,YZcc),(Xa,Cb,YZcd),(Xa,Cb,YZce),(Xa,Cb,YZcf),(Xa,Cb,YZcg),(Xa,Cb,YZch),(Xa,Cb,YZci),(Xa,Cb,YZcj),(Xa,Cb,YZck),(Xa,Cb,YZcl),(Xa,Cb,YZcm),(Xa,Cb,YZcn),(Xa,Cb,YZco),(Xa,Cb,YZcp),(Xa,Cb,YZcq),(Xa,Cb,YZcr),(Xa,Cb,YZcs),(Xa,Cb,YZct),(Xa,Cb,Ycu),(Xa,Cb,YZcv),(Xa,Cb,YZcw),(Xa,Cb,YZcx),(Xa,Cb,YZey),(Xa,Cb,YZcz),(Xa,Cb,YZda),(Xa,Cb,YZdb),(Xa,Cb,YZdc),(Xa,Cb,YZdd),(Xa,Cb,YZde),(Xa,Cb,YZdf),(Xa,Cb,YZdg),(Xa,Cb,YZdh),(Xa,Cb,YZdi),(Xa,Cb,YZdj),(Xa,Cb,YZdk),(Xa,Cb,YZdl),(Xa,Cb,YZdm),(Xa,Cb,YZdn),(Xa,Cb,YZdo),(Xa,Cb,YZdp),(Xa,Cb,YZdq),(Xa,Cb,YZdr),(Xa,Cb,YZds),(Xa,Cb,Yzdt),(Xa,Cb,YZdu),(Xa,Cb,YZdv),(Xa,Cb,YZdw),(Xa,Cb,YZdx),(Xa,Cb,YZdy),(Xa,Cb,YZdz),(Xa,Cb,YZea),(Xa,Cb,YZeb),(Xa,Cb,YZec),(Xa,Cb,YZed),(Xa,Cb,YZee),(Xa,Cb,YZef),(Xa,Cb,YZeg),(Xa,Cb,YZeh),(Xa,Cb,YZei),(Xa,Cb,YZej),(Xa,Cb,YZek),(Xa,Cb,YZel),(Xa,Cb,YZem),(Xa,Cb,YZen),(Xa,Cb,YZeo),(Xa,Cb,YZep),(Xa,Cb,YZeq),(Xa,Cb,YZer),(Xa,Cb,YZes),(Xa,Cb,YZet),(Xa,Cb,YZeu),(Xa,Cb,YZev),(Xa,Cb,YZew),(Xa,Cb,YZex),(Xa,Cb,YZey),(Xa,Cb,YZez),(Xa,Cb,YZfa),(Xa,Cb,YZfb),(Xa,Cb,YZfc),(Xa,Cb,YZfd),(Xa,Cb,YZfe),(Xa,Cb,YZff),(Xa,Cb,YZfg),(Xa,Cb,YZfh),(Xa,Cb,YZfi),(Xa,Cb,YZfj),(Xa,Cb,YZfk),(Xa,Cb,YZfl),(Xa,Cb,YZfm),(Xa,Cb,YZfn),(Xa,Cb,YZfo),(Xa,Cb,YZfp),(Xa,Cb,YZfq),(Xa,Cb,YZfr),(Xa,Cb,YZfs),(Xa,Cb,YZft),(Xa,Cb,YZfu),(Xa,Cb,YZfv),(Xa,Cb,YZfw),(Xa,Cb,YZfx),(Xa,Cb,YZfy),(Xa,Cb,YZfz),(Xa,Cb,YZga),(Xa,Cb,YZgb),(Xa,Cb,YZgc),(Xa,Cb,Y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The invention disclosed herein is also meant to encompass prodrugs ofthe disclosed compounds. Prodrugs are considered to be any covalentlybonded carriers that release the active parent drug in vivo.Non-limiting examples of prodrugs include esters or amides of compoundsof Formulae I, I′, I″, II or II′ having hydroxyalkyl or aminoalkyl as asubstituent, and these can be prepared by reacting such compounds withanhydrides such as succinic anhydride.

The invention disclosed herein is also meant to encompass the disclosedcompounds being isotopically-labelled by having one or more atomsreplaced by an atom having a different atomic mass or mass number.Examples of isotopes that can be incorporated into the disclosedcompounds include isotopes of hydrogen, carbon, nitrogen, oxygen,phosphorous, fluorine and chlorine, such as ²H, ³H, ¹¹C, ¹³c, ¹⁴c, ¹⁵N,¹⁸O, ¹⁷O, ³¹P, ³²P, ³⁵S, ¹⁸F, and ³⁶Cl, respectively, and preferably ³H,¹¹C, and ¹⁴C. Isotopically-labeled compounds of the present inventioncan be prepared by methods known in the art.

The present invention is also directed specifically to ³H, ¹¹C, and ¹⁴ Cradiolabeled compounds of Formula I, I′, I″, II or II′ as well as theirpharmaceutically acceptable salts, prodrugs and solvates, and the use ofany such compounds as radioligands for their binding site on the calciumchannel. For example, one use of the labeled compounds of the presentinvention is the characterization of specific receptor binding. Anotheruse of the labeled compounds of the present invention is an alternativeto animal testing for the evaluation of structure-activityrelationships. For example, the receptor assay may be performed at afixed concentration of a labeled compound of Formula I, I′, I″, II orII′ and at increasing concentrations of a test compound in a competitionassay. For example, tritiated compounds of any of Formula I, I′, I″, IIor II′ can be prepared by introducing tritium into the particularcompound of Formula I, I′, I″, II or II′, for example, by catalyticdehalogenation with tritium. This method may include reacting a suitablyhalogen-substituted precursor of a compound of Formula I, I′, I″, II orII′ with tritium gas in the presence of a suitable catalyst, forexample, Pd/C, in the presence or absence of a base. Other suitablemethods for preparing tritiated compounds can be found in Filer,Isotopes in the Physical and Biomedical Sciences, Vol. 1, LabeledCompounds (Part A), Chapter 6 (1987). ¹⁴C-labeled compounds can beprepared by employing starting materials having a ¹⁴C carbon.

Some of the compounds disclosed herein may contain one or moreasymmetric centers and may thus give rise to enantiomers, diastereomers,and other stereoisomeric forms. The present invention is meant toencompass the uses of all such possible forms, as well as their racemicand resolved forms and mixtures thereof. The individual enantiomers maybe separated according to methods known to those of ordinary skill inthe art in view of the present disclosure. When the compounds describedherein contain olefinic double bonds or other centers of geometricasymmetry, and unless specified otherwise, it is intended that theyinclude both E and Z geometric isomers. All tautomers are intended to beencompassed by the present invention as well.

As used herein, the term “stereoisomers” is a general term for allisomers of individual molecules that differ only in the orientation oftheir atoms in space. It includes enantiomers and isomers of compoundswith more than one chiral center that are not mirror images of oneanother (diastereomers).

The term “chiral center” refers to a carbon atom to which four differentgroups are attached.

The terms “enantiomer” and “enantiomeric” refer to a molecule thatcannot be superimposed on its mirror image and hence is optically activewherein the enantiomer rotates the plane of polarized light in onedirection and its mirror image compound rotates the plane of polarizedlight in the opposite direction

The term “racemic” refers to a mixture of equal parts of enantiomers andwhich mixture is optically inactive.

The term “resolution” refers to the separation or concentration ordepletion of one of the two enantiomeric forms of a molecule.

The terms “a” and “an” refer to one or more.

The invention disclosed herein also encompasses the use of all salts ofthe disclosed compounds, including all non-toxic pharmaceuticallyacceptable salts thereof of the disclosed compounds. Examples ofpharmaceutically acceptable addition salts include inorganic and organicacid addition salts and basic salts. The pharmaceutically acceptablesalts include, but are not limited to, metal salts such as sodium salt,potassium salt, cesium salt and the like; alkaline earth metals such ascalcium salt, magnesium salt and the like; organic amine salts such astriethylamine salt, pyridine salt, picoline salt, ethanolamine salt,triethanolamine salt, dicyclohexylamine salt,N,N′-dibenzylethylenediamine salt and the like; inorganic acid saltssuch as hydrochloride, hydrobromide, hydrofluoride, phosphate, sulfate,nitrate and the like; organic acid salts such as citrate, lactate,tartrate, maleate, fumarate, mandelate, acetate, dichloroacetate,trifluoroacetate, oxalate, formate, succinate, and the like; sulfonatessuch as methanesulfonate, benzenesulfonate, p-toluenesulfonate and thelike; and amino acid salts such as arginate, asparginate, glutamate andthe like.

Acid addition salts can be formed by mixing a solution of the particularcompound of the present invention with a solution of a pharmaceuticallyacceptable non-toxic acid such as hydrochloric acid, fumaric acid,maleic acid, succinic acid, acetic acid, citric acid, tartaric acid,carbonic acid, phosphoric acid, oxalic acid, dichloroacetic acid, andthe like. Basic salts can be formed by mixing a solution of theparticular compound of the present invention with a solution of apharmaceutically acceptable non-toxic base such as sodium hydroxide,potassium hydroxide, choline hydroxide, sodium carbonate and the like.

The invention disclosed herein is also meant to encompass solvates ofthe disclosed compounds. One type of solvate is a hydrate. Solvatestypically do not contribute significantly to the physiological activityor toxicity of the compounds and as such can function as pharmacologicalequivalents.

Some compounds of the present invention may have one or more of thefollowing characteristics:

high affinity of calcium (Ca²⁺) channels, especially N-type calciumchannels,

high selectivity to calcium (Ca²⁺) channels, especially N-type calciumchannels than other channels,

reduced side effect,

high stability

high oral absorbability,

high bioavailability,

low clearance,

easily transfers to brain

long half-life,

long efficacy of a medicine and /or

high protein-unbound fraction.

These compounds are considered useful as blockers of calcium (Ca²⁺)channels, especially N-type calcium channels.

Since compounds of Formula I or I′ are blockers of calcium (Ca²⁺)channels, a number of diseases and conditions mediated by calcium ioninflux can be treated by employing these compounds. Therefore, thepresent invention provides a method of treating, preventing orameliorating stroke, neuronal damage resulting from head trauma,epilepsy, pain (e.g., acute pain, chronic pain, which includes but isnot limited to, neuropathic pain and inflammatory pain, or surgicalpain), migraine, a mood disorder, schizophrenia, a neurodegenerativedisorder (e.g., Alzheimer's disease, amyotrophic lateral sclerosis(ALS), or Parkinson's disease), depression, anxiety, a psychosis,hypertension, or cardiac arrhythmia. In one embodiment, the inventionprovides a method of treating pain. In another embodiment, the type ofpain treated is chronic pain. In another embodiment, the type of paintreated is neuropathic pain. In another embodiment, the type of paintreated is inflammatory pain. In another embodiment, the type of paintreated is acute pain. In each instance, such method of treatment,prevention, or amelioration require administering to an animal in needof such treatment, prevention or amelioration an amount of a compound ofthe present invention that is therapeutically effective in achievingsaid treatment, prevention or amelioration. In one embodiment, theamount of such compound is the amount that is effective as to blockcalcium channels in vivo.

Chronic pain includes, but is not limited to, neuropathic pan,inflammatory pain, postoperative pain, cancer pain, osteoarthritis painassociated with metastatic cancer, trigeminal neuralgia, acute herpeticand postherpetic neuralgia, diabetic neuropathy, causalgia, brachialplexus avulsion, occipital neuralgia, reflex sympathetic dystrophy,fibromyalgia, gout, phantom limb pain, bum pain, and other forms ofneuralgia, neuropathic, and idiopathic pain syndromes.

Chronic somatic pain generally results from inflammatory responses totissue injury such as nerve entrapment, surgical procedures, cancer orarthritis (Brower, Nature Biotechnology 2000; 18: 387-391).

The inflammatory process is a complex series of biochemical and cellularevents activated in response to tissue injury or the presence of foreignsubstances (Levine, Inflammatory Pain, In: Textbook of Pain, Wall andMelzack eds., 3^(rd) ed., 1994). Inflammation often occurs at the siteof injured tissue, or foreign material, and contributes to the processof tissue repair and healing. The cardinal signs of inflammation includeerythema (redness), heat, edema (swelling), pain and loss of function(ibid.). The majority of patients with inflammatory pain do notexperience pain continually, but rather experience enhanced pain whenthe inflamed site is moved or touched. Inflammatory pain includes, butis not limited to, osteoarthritis and rheumatoid arthritis.

Chronic neuropathic pain is a heterogenous disease state with an unclearetiology. In chronic neuropathic pain, the pain can be mediated bymultiple mechanisms. This type of pain generally arises from injury tothe peripheral or central nervous tissue. The syndromes include painassociated with spinal cord injury, multiple sclerosis, post-herpeticneuralgia, trigeminal neuralgia, phantom pain, causalgia, and reflexsympathetic dystrophy and lower back pain. The chronic pain is differentfrom acute pain in that patients suffer the abnormal pain sensationsthat can be described as spontaneous pain, continuous superficialburning and/or deep aching pain. The pain can be evoked by heat-, cold-,and mechano-hyperalgesia or by heat-, cold-, or mechano-allodynia.

Neuropathic pain can be caused by injury or infection of peripheralsensory nerves. It includes, but is not limited to, pain from peripheralnerve trauma, herpes virus infection, diabetes mellitus, causalgia,plexus avulsion, neuroma, limb amputation, and vasculitis. Neuropathicpain is also caused by nerve damage from chronic alcoholism, humanimmunodeficiency virus infection, hypothyroidism, uremia, or vitamindeficiencies. Stroke (spinal or brain) and spinal cord injury can alsoinduce neuropathic pain. Cancer-related neuropathic pain results fromtumor growth compression of adjacent nerves, brain, or spinal cord. Inaddition, cancer treatments, including chemotherapy and radiationtherapy, can also cause nerve injury. Neuropathic pain includes but isnot limited to pain caused by nerve injury such as, for example, thepain from which diabetics suffer.

The present invention is also directed more generally to a method fortreating a disorder responsive to the blockade of calcium channels, andparticularly the selective blockade of N-type calcium channels, in ananimal suffering from said disorder, said method comprisingadministering to the animal an effective amount of a compoundrepresented by any of defined Formula I, I′, I″, II or II′, or apharmaceutically acceptable salt, prodrug or solvate thereof.

The present invention is also directed to the use of a compoundrepresented by any of defined Formula I, I′, I″, II or II′, or apharmaceutically acceptable salt, prodrug or solvate thereof, in themanufacture of a medicament for treating a disorder responsive to theblockade of calcium channels in an animal suffering from said disorder.In one embodiment, the disorder is responsive to the selective blockadeof N-type calcium channels.

Furthermore, the present invention is directed to a method of modulatingcalcium channels, especially N-type calcium channels, in an animal inneed thereof, said method comprising administering to the animal atleast one compound represented by any of defined Formula I, I′, I″, IIor II′, or a pharmaceutically acceptable salt, prodrug or solvatethereof.

The present invention is also directed to the use of a compoundrepresented by any of defined Formula I or I′, or a pharmaceuticallyacceptable salt, prodrug or solvate thereof, in the manufacture of amedicament for modulating calcium channels, especially N-type calciumchannels, in an animal in need thereof.

Synthesis of Compounds

The compounds of the present invention can be prepared in a number ofways well known to those skilled in the art. The compounds of thepresent invention can be synthesized using the methods outlined below,together with methods known in the art of synthetic organic chemistry,or variations thereof as appreciated by those skilled in the art.Preferred methods include, but are not limited to, those describedbelow.

In order to generate compounds of general formula (I) a multi-stepreaction sequence as described in Scheme I can be employed. Herein, apiperidone or the corresponding equivalent (1a), wherein R and p are asdefined above, is reacted with an acid (Z-Y—OH, Y: C═O), wherein Z is asdefined above. Typically the reaction is effected using standard amidecoupling conditions, familiar to one skilled in the art, such asN-ethyldimethylaminopropylcarbodiimide hydrochloride/1-Hydroxybenzotriazole. The acid chloride (Z-Y—Cl, Y: C═O), acidanhydride (Z-Y-Z, Y: C═O) or sulfonyl chloride (Z-Y—Cl, Y: S═O) can alsobe coupled to amine (1a) by using standard conditions, familiar to oneskilled in the art. The resultant ketone (1b) can then be coupled withan O-substituted hydroxylamine (X—W—O—NH₂) or the corresponding salt,e.g. hydrochloric acid salt or trifluoroacetic acid salt, wherein X andW are as defined above, in a suitable solvent such as ethanol, in thepresence of a base such as sodium acetate to generate the desired oxime(I). The O-substituted hydroxylamines (X—W—O—NH₂) are eithercommercially available or can be readily prepared using proceduresfamiliar to one skilled in the art. Non-limiting examples of suchpreparations have been described by e.g. J. N. Kim et al.: SyntheticCommunications, (1992) 22, 1427-1432, H. M. Petrassi et al.: OrganicLetters (2001), 3, 139-142, E. Grochowski, J. Jurczak: Synthesis (1976),682-684, WO02/06213 and WO2005/054179. Typical but non-limitingsynthetic routes to obtain O-substituted hydroxylamines of generalformula (2c) is illustrated in Scheme 2.

Reaction of N-hydroxyphthalimide or N-protected hydroxylamines(G¹-NH—OH; G¹ is an amino protecting group such asN-tert-butoxycarbonyl, N-benzyloxycarbonyl or N-phthalimide) with ahalide or the corresponding equivalent (2a, Hal=Cl, Br, I, OTs etc.)wherein X and W are as defined above, in a suitable solvent in thepresence of a base such as triethylamine,1,8-diazabicyclo[5,4,0]-undec-7-ene (DBU), K₂CO₃ afford intermediates(2b) or (2d) respectively. Alternatively an alcohol (2e) wherein X and Ware as defined above, can be reacted with N-hydroxyphthalimide in aMitsunobu-like reaction in the presence of triphenylphosphine anddiethyl azodicarboxylate (DEAD) or diisopropyl azodicarboxyrate in asuitable solvent such as tetrahydrofuran, affording compounds (2d).Reaction of (2d) with hydrazine monohydrate or methylhydrazine affordsthe desired O-substituted hydroxylamines (2c). Treatment ofintermediates (2b) with acid, e.g. trifluoroacetic acid or hydrochloricacid also yields the desired O-substituted hydroxylamines (2c). TheO-substituted hydroxylamines (2c) can be isolated and used either asfree amines or as the corresponding salts, e.g. hydrochloric acid saltsor trifluoroacetic acid salts.

Alternative ways of preparing some of the compounds of the presentinvention are detailed in Schemes 3 to 10.

wherein R, p, q, X, Y, Z and W are as defined above.

As an alternative to Scheme 1, Scheme 3 employs a hydroxylimine (3a)which can be prepared by similar conditions as described for thegeneration of oximes (I) in Scheme 1. Alkylation of a hydroxylimine (3a)with a halide or the corresponding equivalent (X—W-Hal; Hal=Cl, Br, I,OTs etc.), in a suitable solvent such as N,N-dimethylformamide, in thepresence of a base such as NaH can generate the desired oxime (I).

wherein R, p, q, X, Y, Z and W are as defined above, and G² is a hydroxyprotecting group such as N-tert-butoxycarbonyl, N-benzyloxycarbonyl orN-benzyl.

As an alternative to Scheme 1 and 3, Scheme 4 employs a suitablyprotected piperidone (4a), whereby G²O—C-OG² is, for example,1,3-dioxolane. This can be subjected to alkylation with a halide or thecorresponding equivalent (Z-Y-Hal; Hal=Cl, Br, I, OTs etc.), in asuitable solvent such as acetonitrile, in the presence of a base such asK₂CO₃ to yield a suitably protected alkylated piperidone (4b).

Deprotection can be accomplished using standard conditions, familiar toone skilled in the art. The O-substituted hydroxylamine (X—W—O—NH₂) orthe corresponding hydrochloride can then be coupled to the free ketone(1b) in an analogous manner to previously described in Scheme 1.

wherein R, p, q, X, Y, Z and W are as defined above.

As an alternative to Scheme 1, 3 and 4, in Scheme 5, a piperidone or thecorresponding equivalent (1a), wherein R and p are as defined above, isfirst reacted with an O-substituted hydroxylamine (X—W—O—NH₂) or thecorresponding hydrochloride by similar conditions as described for thegeneration of oximes (I) in Scheme 1. The resultant oxime (5a) can thenbe coupled with an acid (Z-Y—OH, Y: C═O), acid chloride (Z-Y—Cl, Y:C═O), acid anhydride (Z-Y-Z, Y: C═O) or sulfonyl chloride (Z-Y—Cl, Y:S═O) by similar conditions as described for the generation of the ketone(1b) in Scheme 1 to generate the desired oxime (I). A halide or thecorresponding equivalent (Z-Y-Hal; Hal=Cl, Br, I, OTs etc.) can also bereacted with the oxime (5a) by similar conditions as described for thegeneration of the alkylated piperidone (4b) in Scheme 4. The isocyanate,thioisocyanate or the corresponding equivalent can also be coupled tothe oxime (5a) by using standard conditions, familiar to one skilled inthe art.

wherein R, p, q, X, Z, W and G¹ are as defined above, Y═CO or SO₂.

As an alternative to Scheme 1 and 3 to 5, Scheme 6 employs a suitablyprotected piperidone (6a), whereby G¹ is, for example,t-butyloxycarbonyl. This can be coupled with an O-substitutedhydroxylamine (X—W—O—NH₂) or the corresponding hydrochloride by similarconditions as described for the generation of oximes (I) in Scheme 1.Deprotection can be accomplished using standard conditions, familiar toone skilled in the art. The acid (Z-Y—OH, Y: C═O), acid chloride(Z-Y—Cl, Y: C═O), acid anhydride (Z-Y-Z, Y: C═O) or sulfonyl chloride(Z-Y—Cl, Y: SO₂), can be coupled with free amine (6c) in an analogousmanner to previously described in Scheme 1. The isocyanate orthioisocyanate can also be coupled to amine (6c) by using standardconditions, familiar to one skilled in the art.

wherein R, p, q, X, W and G¹ are as defined above, Y is CO or SO₂, andA₁, A₂, A₃ and A₄ are each independently a substituent for “optionallysubstituted lower alkyl” or “optionally substituted lower alkenyl.”

Intermediate amine (6c) can be further utilized to synthesize compoundsof general formula (Ia). An optionally substituted acrylic acid(Z′-Y—OH, Y: C═O), acryl chloride (Z′-Y—Cl, Y: C═O), acrylic anhydride(Z′-Y-Z′, Y: C═O), vinylsulfonyl chloride (Z′-Y—Cl, Y: SO₂) or thecorresponding equivalent can be coupled with free amine (6c) in ananalogous manner to previously described in Scheme 1. The resultingcompound (7a) can react with a nucleophile (A₄-H) such as an amine or analcohol to give the desired oxime (Ia).

wherein R, p, q, X, W and G¹ are as defined above, and B₁, B₂, B₃, B₄and B₅ are each independently a substituent for “optionally substitutedaryl.”

Intermediate amine (6c) can be further utilized to synthesize compoundsof general formula (1b). An optionally substituted acrylic acid(Z′-Y—OH, Y: C═O), acryl chloride (Z′-Y—Cl, Y: C═O), acrylic anhydride(Z′-Y-Z′, Y: C═O), vinylsulfonyl chloride (Z′-Y—Cl, Y: SO₂) or thecorresponding equivalent can be coupled with free amine (6c) in ananalogous manner to previously described in Scheme 1. The resultingcompound (8a) can react with a nucleophile (B₅—H) such as an amine or analcohol to give the desired oxime (1b).

wherein R, p, q, X, W and G¹ are as defined above, C₁ and C₂ are eachindependently a substituent for “optionally substituted heteroaryl” andHal are halogen. Intermediate amine (6c) can also be further utilized tosynthesize compounds of general formula (Ic). Optionally substitutedhalopyridinesulfonyl chloride can be coupled with free amine (6c) in ananalogous manner to previously described in Scheme 1. The resultingcompound (9a) can react with a nucleophile (C₂—H) such as an amine or analcohol to give the desired oxime (Ic).

wherein R, p, q, X, Y and W are as defined above, Y is CO or SO₂, andHal is halogen. Intermediate amine (5a) can be further utilized tosynthesize compounds of general formula (Id). A halogen substituted acid(Hal-CH₂—Y—OH, Y: C═O), acid chloride (Hal-CH₂—Y—Cl, Y: C═O), acidanhydride (Hal-CH₂—Y—CH₂-Hal, Y: C═O), sulfonyl chloride (Hal-CH₂—Y—Cl,Y: S═O) or the corresponding equivalent can be coupled with free amine(5a) in an analogous manner to previously described in Scheme 1. Theresulting compound (10a) can react with a nucleophile (D-H) such as anamine or an alcohol to give the desired oxime (Id).

Testing of Compounds

Representative compounds of the present invention were assessed bycalcium mobilization and/or electrophysiological assays for calciumchannel blocker activity. One aspect of the present invention is basedon the use of the compounds herein described as N-type calcium channelblockers. In one aspect of the present invention, it has been found thatcertain compounds herein described show selectivity as N-type calciumchannel blockers. Based upon this property, these compounds areconsidered useful in treating, preventing, or ameliorating stroke,neuronal damage resulting from head trauma, migraine, epilepsy, a mooddisorder, schizophrenia, a neurodegenerative disorder (such as, e.g.,Alzheimer's disease, ALS, or Parkinson's disease), a psychosis,depression, anxiety, hypertension, or cardiac arrhythmia. The compoundsof the present invention are also expected to be effective in treating,preventing or ameliorating pain, such as acute pain, chronic pain, whichincludes but is not limited to, neuropathic pain and inflammatory painor surgical pain.

More specifically, the present invention is directed to compounds ofFormula I, I′, I″, II or II′ that are blockers of calcium channels.According to the present invention, those compounds having preferredN-type calcium channel blocking properties exhibit an IC₅₀ of about 100μM or less in the calcium mobilization and/or electrophysiologicalassays described herein. Preferably, the compounds of the presentinvention exhibit an IC₅₀ of 10 μM or less. Most preferably, thecompounds of the present invention exhibit an IC₅₀ of about 1.0 μM orless. Compounds of the present invention can be tested for their N-typeand L-type Ca²⁺ channel blocking activity by the following calciummobilization and/or electrophysiological assays.

In one embodiment, compounds useful in the present invention are thoserepresented by any one of Formula I, I′, I″, II or II′ that exhibitselectivity for N-type calcium channels over L-type calcium channels inthe calcium mobilization and/or electrophysiological assays describedherein. The phrase “selectivity for N-type calcium channels over L-typecalcium channels” is used herein to mean that the ratio of an IC₅₀ forL-type channel blocking activity for a compound of the present inventionover an IC₅₀ for N-type channel blocking activity for the same compoundis more than 1, i.e., LTCC IC₅₀/NTCC IC₅₀>1. Preferably, compounds ofthe present invention exhibit an LTCC IC₅₀/NTCC IC₅₀ ratio of about 2 ormore, about 10 or more, about 20 or more, about 30 or more, about 50 ormore, or about 100 or more.

Calcium Mobilization and Electrophysiological Assay Protocols:

Cell maintenance and differentiation. Unless noted otherwise, cellculture reagents were purchased from Mediatech of Hemdon, Md. IMR32cells (American Type Culture Collection, ATCC, Manassas, Va.) wereroutinely cultured in growth medium consisting of minimum essentialmedium containing 10% fetal bovine serum (FBS, Hyclone, Logan, Utah),100 U/mL penicillin, 100 μg/mL streptomycin, 2 mM L-glutamine, 1 mMsodium pyruvate, and 1× MEM non-essential amino acids. 80-90% confluentflasks of cells were differentiated using the following differentiationmedium: Growth medium plus 1 mM dibutyryl cyclic AMP (Sigma, St. Louis,Mo.), and 2.5 μM bromodeoxyuridine (Sigma). Cells were differentiatedfor 8 days by replacing differentiation medium every 2-3 days.

A7r5 (ATCC) cells were maintained and routinely cultured in A7r5 growthmedium consisting of Dulbecco's Modified Eagles Medium containing 10%FBS, 100 U/mL penicillin, 100 μg/mL streptomycin, 4 mM L-glutamine, and0.15% sodium bicarbonate. 80-90% confluent flasks of cells weredifferentiated using the following differentiation medium: A7r5 GrowthMedium plus 1 mM dibutyryl cyclic AMP (Sigma). Cells were differentiatedfor 8 days by replacing differentiation medium every 2-3 days.

Recombinant human embryonal kidney cells (HEK293, ATCC) stablytransfected with either N-type calcium channel (NTCC) subunits (α1b,α2δ, and β3) or L-type calcium channel (LTCC) subunits (α1c, α2δ, andβ1) were routinely cultured in growth medium consisting of Dulbecco'sModified Eagles Medium containing 10% FBS, 100 U/mL penicillin, 100μg/mL streptomycin, 4 mM L-glutamine, 500 μg/mL geneticin (G418), 20μg/mL Blasticidin S (InVivogen, San Diego, Calif.) and 500 μg/mL zeocin(InVivogen).

FLIPR Calcium Mobilization Assay for N-type Calcium Channel. One dayprior to performing this assay, differentiated IMR32 cells were treatedwith 1× CellStripper, and seeded on poly-D-lysine-coated 96-wellclear-bottom black plates (Becton Dickinson, Franklin Lakes, N.J.) at200,000 cells/well. On the day of the assay, the cell plates were washedwith IMR32 buffer (127 mM NaCl, 1 mM KCl, 2 mM MgCl₂, 700 μM NaH₂PO₄, 5mM CaCl₂, 5 mM NaHCO₃, 8 mM HEPES, 10 mM glucose, pH 7.4), thenpre-stimulated with KCl and loaded as follows: 0.05 mL of IMR32 buffer,0.05 mL of each compound tested diluted in IMR32 buffer containing 20 μMnitrendipine (Sigma), and 0.1 mL KCl dissolved in IMR32 buffer, plusFluo-4 were added (3 μM final concentration, Molecular Probes, Eugene,Oreg.). Final test compound concentrations ranged from about 846 pM toabout 17 μM, final nitrendipine concentration was 5 μM, and final KClconcentration was 90 mM. After 1 hour, the cells were washed twice with0.05 mL of each compound tested in nitrendipine-containing IMR32 buffer(no KCl or Fluo-4), and then replaced with 0.1 mL of each compoundtested in nitrendipine-containing IMR32 buffer. Plates were thentransferred to a Fluorimetric imaging Plate Reader (FLIPR⁹⁶, MolecularDevices, Inc., Sunnyvale, Calif.) for assay. The FLIPR measured basalFluo-4 fluorescence for 315 seconds (i.e., 5 minutes and 15 seconds),then added 0.1 mL KCl agonist dissolved in IMR32 buffer and measuredfluorescence for another 45 seconds. Final test compound concentrationson the cells after FLIPR read ranged from about 846 pM to about 17 μM,final nitrendipine concentration was 5 μM, and final KCl concentrationwas 90 mM. Data were collected over the entire time course and analyzedusing Excel, Graph Pad Prism (version 3.02, Graph Pad, San Diego,Calif.), or an in-house non-linear regression analysis software.

FLIPR Calcium Mobilization Assay for L-type Calcium Channel. One dayprior to performing this assay, HEK293 cells stably expressingrecombinant rat L-type calcium channel (LTCC) subunits (α1c, α2δ, andβ1) were trypsinized, then seeded on poly-D-lysine-coated 96-wellclear-bottom black plates (Becton Dickinson, Franklin Lakes, N.J.) at75,000 cells/well. On the day of the assay, the plates were washed withLTCC wash buffer (127 mM NaCl, 2 mM MgCl₂, 700 μM NaH₂PO₄, 5 nM CaCl₂, 5mM NaHCO₃, 8 mM HEPES, 10 mM glucose, pH 7.4), then loaded with 0.1 mLof LTCC wash buffer containing Fluo-4 (3 μM final concentration,Molecular Probes, Eugene, Oreg.). After 1 hour, the cells were washedwith 0.1 mL LTCC wash buffer and resuspended in 0.05 mL LTCC assaybuffer (same composition as LTCC wash buffer). Plates were thentransferred to a FLIPR⁹⁶ for assay. The FLIPR measured basal Fluo-4fluorescence for 15 seconds, then added 0.05 mL of each compound testeddiluted in LTCC assay buffer at final concentrations ranging from about846 pM to about 17 μM. Fluo-4 fluorescence was then measured for 5minutes. 0.1 mL KCl agonist dissolved in LTCC assay buffer was thenadded to the cells to produce a final concentration of 90 mM KCl, andfluorescence was measured for another 45 seconds. Data were collectedover the entire time course and analyzed using Excel, Graph Pad Prism,or an in-house regression analysis software.

Alternative FLIPR Calcium Mobilization Assay for L-Type Calcium Channel.

Alternatively, the following cell line and procedure may be used for theFLIPR calcium mobilization assay for L-type calcium channel. One dayprior to performing this assay, differentiated A7r5 cells aretrypsinized, then seeded on tissue culture treated 96-well clear-bottomblack plates (Becton Dickinson, Franklin Lakes, N.J.) at a dilution of1:1 from a confluent T150 cm² flask. On the day of the assay, the platesare washed with A7r5 wash buffer (127 mM NaCl, 2 mM MgCl₂, 700 μMNaH₂PO₄, 5 mM CaCl₂, 5 mM NaHCO₃, 8 mM HEPES, 10 mM glucose, pH 7.4),then loaded with 0.1 mL of A7r5 wash buffer containing Fluo-4 (3 μMfinal concentration, Molecular Probes, Eugene, Oreg.). After 1 hour, thecells are washed with 0.1 mL A7r5 wash buffer and resuspended in 0.05 mLA7r5 assay buffer that is composed of A7r5 wash buffer plus 50 μMvalinomycin (Sigma). Plates are then transferred to a FLIPR⁹⁶ for assay.The FLIPR measures basal Fluo-4 fluorescence for 15 seconds, then adds0.05 mL of each compound tested diluted in A7r5 assay buffer at finalconcentrations ranging from about 846 pM to about 17 μM. Fluo-4fluorescence is then measured for 5 minutes. 0.1 mL KCl agonistdissolved in A7r5 assay buffer is then added to the cells to produce afinal concentration of 90 mM KCl, and fluorescence was measured foranother 45 seconds. Data were collected over the entire time course andanalyzed using Excel, Graph Pad Prism, or an in-house regressionanalysis software.

Cloning of N- and L-type calcium channel subunit open reading framecDNAs. Five cDNAs encoding subunits of the rat N- or L-type calciumchannels were cloned by PCR amplification in order to reconstitutefunctional channels in a heterologous system. These were the alpha1b(α1b), beta1 (β1), beta3 (β3), alpha2delta (α2δ), and alpha1c (α1c)subunit cDNAs. The alpha1b subunit cDNA has been described by Dubel etal. in Proc. Natl. Acad. Sci. U.S.A 89: 5058-5062 (1992). The beta1subunit cDNA has been described by Pragnell et al. in FEBS Lett. 291:253-258 (1991). The beta3 subunit cDNA has been described by Castellanoet al. in J. Biol. Chem. 268: 12359-12366 (1993). The alpha2deltasubunit cDNA has been described by Kim et al. in Proc. Natl. Acad. Sci.U.S.A. 89: 3251-3255 (1992). The alpha1c subunit cDNA has been describedby Koch et al. in J. Biol. Chem. 265: 17786-17791 (1990).

The 7.0 kb cDNA containing the entire α1b open reading frame (ORF) wasPCR amplified as two overlapping cDNA fragments, i.e., a 2.7 kb 5′fragment and a 4.4 kb 3′ fragment. The 5′ fragment was amplified fromrat brain cDNA using primers 1 (SEQ ID NO:1, TABLE 1) and 2 (SEQ IDNO:2, TABLE 1), and the 3′ fragment was amplified from rat spinal cordcDNA using primers 3 (SEQ ID NO:3, TABLE 1) and 4 (SEQ ID NO:4, TABLE1). The two fragments were joined by ligation at a common restrictionsite to create the entire 7.0 kb cDNA. This ORF encodes the proteinisoform generated by alternative splicing termed “+A ΔSFMG ΔET”according to the nomenclature of Lin et al. (Neuron 18: 153-166 (1997)).The entire cDNA was sequenced with redundant coverage on both strands.The cDNA was then inserted into the mammalian expression vectorpcDNA6.2DEST (Invitrogen, Carlsbad Calif.) by homologous recombinationusing the Gateway system (Invitrogen).

The 1.8 kb cDNA encoding the β1 subunit, the 1.45 cDNA encoding thebeta3 subunit, and the 3.3 kb cDNA encoding the alpha2delta subunit werecloned by PCR amplification from rat spinal cord cDNA (β1) or brain cDNA(β3, α2δ). Primers 5 (SEQ ID NO:5, TABLE 1) and 6 (SEQ ID NO:6, TABLE 1)were used for the β1 cDNA amplification; primers 7 (SEQ ID NO:7,TABLE 1) and 8 (SEQ ID NO:8, TABLE 1) were used for the β3 cDNAamplification; and primers 9 (SEQ ID NO:9, TABLE 1) and 10 (SEQ IDNO:10, TABLE 1) were used for the α2δ cDNA amplification. PCR productswere subcloned and fully sequenced on both strands. Clones matching thereference sequence (β1: NM_(—)017346; β3: NM_(—)012828; α2δ: M86621) andthe gene's GenBank rat genomic DNA sequences were recombined into themammalian expression vector pcDNA3.2DEST (β1, β3) or pcDNA3.1-Zeo (α2δ),which had been modified to a vector compatible with the Gatewayrecombination system using the Gateway vector adaptor kit (Invitrogen).Proper recombination was confirmed by sequencing of recombinogenicregions. For β3 expression vector, proper protein expression wasconfirmed by Western blot analysis of lysates of transfected HEK293cells using a rabbit polyclonal antiserum directed against the rat β3subunit (USA Biological).

The 6.5 kb cDNA encoding the L-type calcium channel α1c subunit wascloned by PCR amplification from rat heart cDNA using primers 11 (SEQ IDNO: 11, TABLE 1) and 12 (SEQ ID NO:12, TABLE 1). The PCR fragment wassubcloned and fully sequenced on both strands to confirm its identity. Aclone matching consensus reference sequence M59786 and rat genomic DNAsequences was recombined into the mammalian expression vectorpcDNA6.2DEST. Sequences around the recombinogenic region were sequencedto confirm accurate recombination into the expression vector.

TABLE 1 SEQ ID PRIMER SEQUENCE NO. CACC ATG GTC CGC TTC GGG GAC 1 CCGTTC AGT GGC CTC CTC C 2 C TAG CAC CAG TGA TCC TGG TCTG 3 AGT GCG TTG TGAGCG CAG TA 4 CAC CAT GGT CCA GAA GAG CGG 5 TCTCAGCGGATGTAGACGCCT 6 CACCAT GTA TGA CGA CTC CTA C 7 GGT GGT CAG TAG CTG TCC TTA GG 8 CAC CAT GGCTGC TGG CTG CCT 9 AGA GGG TCA CCA TAG ATA GTG TCT G 10CACCATGATTCGGGCCTTCGCT 11 AGCCTGCGGACTACAGGTTGCTGAC 12

N-type Recombinant Cell Line Development. N-type calcium channelexpressing HEK-293 cells were created in two stages. Stage 1 was createdas follows. The rat α1b, and β3 cDNA expression constructs (2.5 μg each)were co-transfected into human embryonic kidney (HEK-293) cells byLipofectamine Plus reagent (Invitrogen), as per manufacturer'sinstructions. 24 hours later, cells were split in limiting dilution intomultiple 96-well plates in selection media containing 20 μg/mLblasticidin and 500 μg/mL geneticin, and incubated for 3 weeks at 37°C., 5% CO₂, 95% humidity. Plates containing ≦1 clone per well werecultured until wells positive for single clones were confluent.Individual clones were then arrayed into columns of a destination96-well plate, and partly split into 6-well plates for culturemaintenance. Array plates were washed once with IMR32 buffer and cellsloaded for 1 hour with 0.1 mL of IMR32 buffer containing Fluo-4 (3 μMfinal concentration, Molecular Probes). Then they were washed twice with0.1 mL of IMR32 buffer, and replaced with 0.1 mL IMR32 buffer. Plateswere then transferred to a FLIPR⁹⁶ for assay. The FLIPR they were washedtwice with 0.1 mL of IMR32 buffer, and replaced with 0.1 mL dissolved inIMR32 buffer and measured fluorescence for another 45 seconds. Final KClconcentration was 90 mM. Data were collected over the entire time courseand analyzed using Excel, Graph Pad Prism, or Activity Base (version5.1, IDBS, Parsippany, N.J.) software. The clone with the greatestsignal-to-noise ratio, best stability of response with passage number,and best adhesion to PDL precoated plates (Becton Dickinson) wasexpanded, characterized and used for stage 2 cell line development.

Stage 2 of N-type cell line development was carried out as follows. Therat α2δ cDNA expression construct (5 μg each) was transfected into thestage 1 N-type clonal cell line by Lipofectamine Plus reagent(Invitrogen), as per manufacturer's instructions. 24 hours later, cellswere split in limiting dilution into multiple 96-well plates inselection media containing 20 μg/mL blasticidin, 500 μg/mL geneticin,and 250 μg/mL zeocin and incubated for 3 weeks at 37° C., 5% CO₂, 95%humidity. Plates containing ≦1 clone per well were cultured and handledaccording to the same steps and procedures described above for the stage1 cell line. The three clones with the greatest signal-to-noise, beststability of response with passage number, and best adhesion to PDLprecoated plates (Becton Dickinson) were expanded, characterized andtested in electrophysiology for the best current size, N-typepharmacology, N-type characteristic current-voltage relationship andkinetics as described below.

L-type Recombinant Cell Line Development. L-type calcium channelexpressing HEK-293 cells were created in two stages. Stage 1 was createdas follows. The rat α1c, and β1 cDNA expression constructs (2.5 μg each)were co-transfected into human embryonic kidney (HEK-293) cells byLipofectamine Plus reagent (Invitrogen), as per manufacturer'sinstructions. 24 hours later, cells were split in limiting dilution intomultiple 96-well plates in selection media containing 20 μg/mLblasticidin and 500 μg/mL geneticin, and incubated for 3 weeks at 37°C., 5% CO₂, 95% humidity. Plates containing ≦1 clone per well werecultured until wells positive for single clones were confluent.Individual clones were then arrayed into columns of a destination96-well plate, and partly split into 6-well plates for culturemaintenance. Array plates were washed once with LTCC wash (or assay)buffer and cells loaded for 1 hour with 0.1 mL of LTCC buffer containingFluo-4 (3 μM final concentration, Molecular Probes). Then they werewashed twice with 0.1 mL of LTCC buffer, and replaced with 0.1 mL LTCCbuffer. Plates were then transferred to a FLIPR⁹⁶ for assay. The FLIPRmeasured basal Fluo-4 fluorescence for 315 seconds, then added 0.1 mLKCl agonist dissolved in LTCC buffer and measured fluorescence foranother 45 seconds. Final KCl concentration was 90 mM. Data werecollected over the entire time course and analyzed using Excel, GraphPad Prism, or Activity Base software. The clone with the greatestsignal-to-noise ratio, best stability of response with passage number,and best adhesion to PDL precoated plates (Becton Dickinson) wasexpanded, characterized and used for stage 2 cell line development.

Stage 2 of L-type cell line development was carried out as follows. Therat α2δ cDNA expression construct (5 μg each) was transfected into thestage 1 L-type clonal cell line by Lipofectamine Plus reagent(Invitrogen), as per manufacturer's instructions. 24 hours later, cellswere split in limiting dilution into multiple 96-well plates inselection media containing 20 μg/mL blasticidin, 500 μg/mL geneticin,and 250 μg/mL zeocin and incubated for 3 weeks at 37° C., 5% CO₂, 95%humidity. Plates containing ≦1 clone per well were cultured and handledaccording to the same steps and procedures described above for the stage1 cell line. The three clones with the greatest signal-to-noise, beststability of response with passage number, and best adhesion to PDLprecoated plates (Becton Dickinson) were expanded and characterized.

N-type Electrophysiology in Recombinant Cells. For electrophysiologicalrecording, the cells expressing α1b, β3 and α2δ subunits were seeded on35-mm culture Petri dishes at a density of approximately 10⁴ cells/dishand kept in an incubator for up to three days for subsequent recordings.For recordings, the dishes were positioned on the stage of an invertedmicroscope (Nikon, Eclipse E600, Japan) and superfused with a bathsolution comprised of BaCl₂ (11 mM), MgCl₂ (1.5 mM), HEPES (10 mM), TEAchloride (120 mM), glucose (10 mM) adjusted to pH 7.4 with KOH.Whole-cell voltage-clamp recordings were made using conventionalpatch-clamp techniques (Hamill et al., Pfluegers Arch. 391: 85-100(1981)) at room temperature (22-24° C.). The patch-clamp pipettes werepulled from WPI, thick-walled borosilicate glass (WPI, Sarasota, Fla.).Currents were recorded using an Axopatch 200A amplifier (AxonInstruments, Union City, Calif.) and were leak-subtracted (P/4),low-pass filtered (1 kHz, 4-pole Bessel), digitized (20-50-μsintervals), and stored using Digidata 1200 B interface andPclamp8.0/Clampex software (Axon Instruments, Union City, Calif.). Thepipettes were back-filled with internal solution containing CsCl (110mM), MgCl₂ (3 mM), EGTA (3 mM), HEPES (40 mM), Mg-ATP (4 mM), Na₂GTP(0.5 mM), and adjusted to pH 7.2 with CsOH. The pipette resistanceranged from 2 to 3 MOhm and was compensated by 75-80% by the built-inelectronic circuitry.

Currents were elicited by stepping from a holding potential of −90 mV to0 mV for 20 ms every 20 sec. At the −90 mV membrane voltage about 50% ofchannels were in the inactivated state, and thus contact with a blockerwould involve interaction with both resting and inactivated channels.Every drug was applied at 3 to 4 concentrations increasing in acumulative manner. Fractional inhibition levels in steady-state wereused to draw the partial inhibition concentration curves to get the IC₅₀(i.e. concentration causing 50% reduction in the size of the response)values at −90 mV. Stock solutions of each test compound were preparedusing DMSO. Serial dilutions to desired concentrations were done withbath solution; concentration of DMSO in final solutions was 0.1%. Drugswere applied by gravity flow using a plane multi-barrel array shooterpositioned 0.5 mm apart from the cell.

All curve fittings were carried out using Origin software (version 5.0,Microcal). A Hill equation was fit to the concentration-inhibitioncurves to determine IC₅₀ values.

N-type Electrophysiology in Neuronal Cells. To determine dissociationconstants in resting versus inactivated state for N-type calciumchannels, neuronal cells that endogenously express N-type calciumchannels can be used. For electrophysiological recording, the neuronalcells expressing N-type calcium channels are seeded on 35-mm culturePetri dishes at a density of approximately 10⁴ cells/dish and kept in anincubator for up to three days for subsequent recordings. Forrecordings, the dishes are positioned on the stage of an invertedmicroscope (Nikon, Eclipse E600, Japan) and superfused with a bathsolution comprised of BaCl₂ (11 mM), MgCl₂ (1.5 mM), HEPES (10 mM), TEAchloride (120 mM), glucose (10 mM) adjusted to pH 7.4 with KOH.Whole-cell voltage-clamp recordings are made using conventionalpatch-clamp techniques (Hamill et al., Pfluegers Arch. 391: 85-100(1981)) at room temperature (22-24° C.). The patch-clamp pipettes arepulled from WPI, thick-walled borosilicate glass (WPI, Sarasota, Fla.).Currents are recorded using an Axopatch 200A amplifier (AxonInstruments, Union City, Calif.) and leak-subtracted (P/4), low-passfiltered (1 kHz, 4-pole Bessel), digitized (20-50-μs intervals), andstored using Digidata 1200 B interface and Pclamp8.0/Clampex software(Axon Instruments, Union City, Calif.). The pipettes are back-filledwith internal solution containing CsCl (1 10 mM), MgCl₂ (3 mM), EGTA (3mM), HEPES (40 mM), Mg-ATP (4 mM), Na₂GTP (0.5 mM), and adjusted to pH7.2 with CsOH. The pipette resistance ranges from 2 to 3 MOhm and iscompensated by 75-80% by the built-in electronic circuitry.

Currents are elicited by stepping from a holding potential of −90 mV to0 mV for 20 ms every 10 sec. At the −90 mV membrane voltage a proportionof channels is in the inactivated state, and thus contact with a blockerwould involve interaction with both resting and inactivated channels.This protocol is used as a first tier screen. For dissection of twocomponents of inhibition (resting block with the apparent dissociationconstant K_(r) and inactivated state block with K_(i)), steady-stateinactivation curves are collected using a double-pulse protocol.Three-second long depolarizing pre-pulse incrementing in 10 mV steps isfollowed by a 10 ms test pulse to 0 mV. Stock solutions of each testcompound are prepared using DMSO. Serial dilutions to desiredconcentrations are done with bath solution; concentration of DMSO infinal solutions is 0.1%. Drugs are applied by gravity flow using a planemulti-barrel array shooter positioned ˜1 mm apart from the cell.

All curve fittings can be carried out using Origin software (version5.0, Microcal). A Hill equation is used to fit theconcentration-response curves and to determine IC₅₀ values. A Boltzmanequation is used to fit inactivation curves, returning half-inactivationvoltage, V_(0.5), slope p and the amplitude of current at the mostnegative voltage where eventually all channels are in the resting state.These parameters are used to calculate the apparent dissociationconstants: K_(r)=((Ab/Ac)/(1−(Ab/Ac))*[b]) where [b] is the drugconcentration, Ac is the maximum test current amplitude in controlconditions and Ab is the maximum test current amplitude in the presenceof a blocker; K_(i)=[b]/((exp(−(dx/p))*(1+([b]/K_(r)))−1) where dx isthe difference between half-inactivation voltage V_(0.5) in the presenceand absence of drug and p is the slope.

In Vivo Pharmacology

The compounds of the present invention can be tested for in vivoanticonvulsant activity after i.v., p.o., or i.p. injection using any ofa number of anticonvulsant tests in mice, including the maximumelectroshock seizure test (MES). Maximum electroshock seizures areinduced in male NSA mice weighing between 15-20 g and in maleSprague-Dawley rats weighing between 200-225 g by application of current(for mice: 50 mA, 60 pulses/sec, 0.8 msec pulse width, 1 sec duration,D.C.; for rats: 99 mA, 125 pulses/sec, 0.8 msec pulse width, 2 secduration, D.C.) using a Ugo Basile ECT device (Model 7801). Mice arerestrained by gripping the loose skin on their dorsal surface andsaline-coated corneal electrodes are held lightly against the twocorneae. Rats are allowed free movement on the bench top and ear-clipelectrodes are used. Current is applied and animals are observed for aperiod of up to 30 seconds for the occurrence of a tonic hindlimbextensor response. A tonic seizure is defined as a hindlimb extension inexcess of 90 degrees from the plane of the body. Results can be treatedin a quantal manner.

The compounds can be tested for their antinociceptive activity in theformalin model as described in Hunskaar, S., O. B. Fasmer, and K. Hole,J. Neurosci. Methods 14: 69-76 (1985). Male Swiss Webster NIH mice(20-30 g; Harlan, San Diego, Calif.) can be used in all experiments.Food is withdrawn on the day of experiment. Mice are placed inPlexiglass jars for at least 1 hour to acclimate to the environment.Following the acclimation period mice are weighed and given either thecompound of interest administered i.p. or p.o., or the appropriatevolume of vehicle (10% Tween-80) as control. Fifteen minutes after thei.p. dosing, and 30 minutes after the p.o. dosing mice are injected withformalin (20 μL of 5% formaldehyde solution in saline) into the dorsalsurface of the right hind paw. Mice are transferred to the Plexiglassjars and monitored for the amount of time spent licking or biting theinjected paw. Periods of licking and biting are recorded in 5-minuteintervals for 1 hour after the formalin injection. All experiments aredone in a blinded manner during the light cycle. The early phase of theformalin response is measured as licking/biting between 0-5 minutes, andthe late phase is measured from 15-50 minutes. Differences betweenvehicle and drug treated groups can be analyzed by one-way analysis ofvariance (ANOVA). A P value<0.05 is considered significant. Compoundsare considered to be efficacious for treating acute and chronic pain ifthey have activity in blocking both the early and second phase offormalin-induced paw-licking activity.

Compounds can be tested for their potential to treat chronic pain (i.e.,antiallodynic and antihyperalgesic activities) using the Chung model ofperipheral neuropathy (Kim and Chung, Pain 50: 355-363 (1992)). MaleSprague-Dawley rats weighing between 200-225 g are anesthetized withhalothane (1-3% in a mixture of 70% air and 30% oxygen), and their bodytemperature controlled during anesthesia through use of a homeotherrnicblanket. A 2-cm dorsal midline incision is then made at the L5 and L6level, and the para-vertebral muscle groups retracted bilaterally. L5and L6 spinal nerves are then exposed, isolated, and tightly ligatedwith 6-0 or 7-0 silk suture. A sham operation is performed exposing thecontralateral L5 and L6 spinal nerves, without ligating, as a negativecontrol.

Tactile Allodynia: Sensitivity to non-noxious mechanical stimuli can bemeasured in animals to assess tactile allodynia. Rats are transferred toan elevated testing cage with a wire mesh floor and allowed to acclimatefor five to ten minutes. A series of von Frey monofilaments are appliedto the plantar surface of the hindpaw to determine the animal'swithdrawal threshold. The first filament used possesses a bucklingweight of 9.1 gms (0.96 log value) and is applied up to five times tosee if it elicits a withdrawal response. If the animal has a withdrawalresponse, then the next lightest filament in the series would be appliedup to five times to determine if it also could elicit a response. Thisprocedure is repeated with subsequent lesser filaments until there is noresponse and the identity of the lightest filament that elicits aresponse is recorded. If the animal does not have a withdrawal responsefrom the initial 9.1 gms filament, then subsequent filaments ofincreased weight are applied until a filament elicits a response and theidentity of this filament is recorded. For each animal, threemeasurements are made at every time point to produce an averagewithdrawal threshold determination. Tests can be performed prior to, andat 1, 2, 4 and 24 hours post drug administration.

Mechanical Hyperalgesia: Sensitivity to noxious mechanical stimuli canbe measured in animals using the paw pressure test to assess mechanicalhyperalgesia. In rats, hind paw withdrawal thresholds (“PWT”), measuredin grams, in response to a noxious mechanical stimulus are determinedusing an analgesymeter (Model 7200, commercially available from UgoBasile of Italy), as described in Stein (Biochemistry & Behavior 31:451-455 (1988)). The rat's paw is placed on a small platform, and weightis applied in a graded manner up to a maximum of 250 grams. The endpointis taken as the weight at which the paw is completely withdrawn. PWT isdetermined once for each rat at each time point. PWT can be measuredonly in the injured paw, or in both the injured and non-injured paw. Inone non-limiting embodiment, mechanical hyperalgesia associated withnerve injury induced pain (neuropathic pain) can be assessed in rats.Rats are tested prior to surgery to determine a baseline, or normal,PWT. Rats are tested again 2 to 3 weeks post-surgery, prior to, and atdifferent times after (e.g. 1, 3, 5 and 24 hr) drug administration. Anincrease in PWT following drug administration indicates that the testcompound reduces mechanical hyperalgesia.

Pharmaceutical Compositions

Although a compound of the present invention may be administered to amammal in the form of a raw chemical without any other componentspresent, the compound is preferably administered as part of apharmaceutical composition containing the compound combined with asuitable pharmaceutically acceptable carrier. Such a carrier can beselected from pharmaceutically acceptable excipients and auxiliaries.Compositions within the scope of the present invention include allcompositions where a compound of the present invention is combined witha pharmaceutically acceptable carrier. In a preferred embodiment, thecompound is present in the composition in an amount that is effective toachieve its intended therapeutic purpose. While individual needs mayvary, a determination of optimal ranges of effective amounts of eachcompound is within the skill of the art. Typically, the compounds may beadministered to mammal, e.g. human, orally at a dose of from about0.0025 to about 1500 mg per kg body weight of the mammal, or anequivalent amount of a pharmaceutically acceptable salt thereof, per dayto treat the particular disorder. A useful oral dose of a compound ofthe present invention administered to a mammal is from about 0.0025 toabout 50 mg per kg body weight of the mammal, or an equivalent amount ofthe pharmaceutically acceptable salt thereof. For intramuscularinjection, the dose is typically about one-half of the oral dose.

A unit oral dose may comprise from about 0.01 to about 50 mg, andpreferably about 0.1 to about 10 mg, of the compound. The unit dose canbe administered one or more times daily as one or more tablets, eachcontaining from about 0.01 to about 50 mg of the compound, or anequivalent amount of a pharmaceutically acceptable salt or solvatethereof.

In one embodiment, a pharmaceutical composition of the present inventioncan be administered orally and is formulated into tablets, dragees,capsules or an oral liquid preparation.

Alternatively, a pharmaceutical composition of the present invention canbe administered rectally, and is formulated in suppositories.

Alternatively, a pharmaceutical composition of the present invention canbe administered by injection.

Alternatively, a pharmaceutical composition of the present invention canbe administered transdermally.

Alternatively, a pharmaceutical composition of the present invention canbe administered by inhalation or by intranasal administration.

Alternatively, a pharmaceutical composition of the present invention canbe administered by the intravaginal route.

A pharmaceutical composition of the present invention can contain fromabout 0.01 to 99 percent by weight, and preferably from about 0.25 to 75percent by weight, of active compound(s).

The present methods of the invention, such as the method for treating,preventing, or ameliorating a disorder responsive to the blockade ofcalcium channels in an animal in need thereof, can further compriseadministering the second therapeutic agent to the animal beingadministered a compound of Formula I, I′, I″, II or II′. In oneembodiment, the second therapeutic agent is administered in an effectiveamount. Effective amounts of the other therapeutic agents are known tothose skilled in the art. However, it is well within the skilledartisan's purview to determine the other therapeutic agent's optimaleffective-amount range. In one embodiment of the invention, whereanother therapeutic agent is administered to an animal, the effectiveamount of the compound of the present invention is less than itseffective amount would be where the other therapeutic agent is notadministered. In this case, without being bound by theory, it isbelieved that compounds of the present invention and the othertherapeutic agent act synergistically to treat, prevent, or ameliorate adisorder or condition.

The second therapeutic agent can be, but is not limited to, an opioidagonist, a non-opioid analgesic, a non-steroidal anti-inflammatoryagent, an antimigraine agent, a Cox-II inhibitor, a β-adrenergicblocker, an anticonvulsant, an antidepressant, an anticancer agent, anagent for treating addictive disorder, an agent for treating Parkinson'sdisease and parkinsonism, an agent for treating anxiety, an agent fortreating epilepsy, an agent for treating a seizure, an agent fortreating a stroke, an agent for treating a pruritic condition, an agentfor treating psychosis, an agent for treating ALS, an agent for treatinga cognitive disorder, an agent for treating a migraine, an agent fortreating vomiting, an agent for treating dyskinesia, or an agent fortreating depression, and mixtures thereof.

Examples of useful opioid agonists include, but are not limited to,alfentanil, allylprodine, alphaprodine, anileridine, benzylmorphine,bezitramide, buprenorphine, butorphanol, clonitazene, codeine,desomorphine, dextromorarmide, dezocine, diampromide, diamorphone,dihydrocodeine, dihydromorphine, dimenoxadol, dimepheptanol,dimethylthiambutene, dioxaphetyl butyrate, dipipanone, eptazocine,ethoheptazine, ethylmethylthiambutene, ethylmorphine, etonitazene,fentanyl, heroin, hydrocodone, hydromorphone, hydroxypethidine,isomethadone, ketobemidone, levorphanol, levophenacylmorphan,lofentanil, meperidine, meptazinol, metazocine, methadone, metopon,morphine, myrophine, nalbuphine, narceine, nicomorphine, norlevorphanol,normethadone, nalorphine, normorphine, norpipanone, opium, oxycodone,oxymorphone, papaveretum, pentazocine, phenadoxone, phenomorphan,phenazocine, phenoperidine, piminodine, piritramide, proheptazine,promedol, properidine, propiram, propoxyphene, sufentanil, tilidine,tramadol, pharmaceutically acceptable salts thereof, and mixturesthereof.

In certain embodiments, the opioid agonist is selected from codeine,hydromorphone, hydrocodone, oxycodone, dihydrocodeine, dihydromorphine,morphine, tramadol, oxymorphone, pharmaceutically acceptable saltsthereof, and mixtures thereof. Examples of useful non-opioid analgesicsinclude non-steroidal anti-inflammatory agents, such as aspirin,ibuprofen, diclofenac, naproxen, benoxaprofen, flurbiprofen, fenoprofen,flubufen, ketoprofen, indoprofen, piroprofen, carprofen, oxaprozin,pramoprofen, muroprofen, trioxaprofen, suprofen, aminoprofen,tiaprofenic acid, fluprofen, bucloxic acid, indomethacin, sulindac,tolmetin, zomepirac, tiopinac, zidometacin, acemetacin, fentiazac,clidanac, oxpinac, mefenamic acid, meclofenamic acid, flufenamic acid,niflumic acid, tolfenamic acid, diflurisal, flufenisal, piroxicam,sudoxicam, isoxicam, and pharmaceutically acceptable salts thereof, andmixtures thereof. Examples of other suitable non-opioid analgesicsinclude the following, non limiting, chemical classes of analgesic,antipyretic, nonsteroidal antiinflammatory drugs: salicylic acidderivatives, including aspirin, sodium salicylate, choline magnesiumtrisalicylate, salsalate, diflunisal, salicylsalicylic acid,sulfasalazine, and olsalazin; para aminophennol derivatives includingacetaminophen and phenacetin; indole and indene acetic acids, includingindomethacin, sulindac, and etodolac; heteroaryl acetic acids, includingtolmetin, diclofenac, and ketorolac; anthranilic acids (fenamates),including mefenamic acid, and meclofenamic acid; enolic acids, includingoxicams piroxicam, tenoxicam), and pyrazolidinediones (phenylbutazone,oxyphenthartazone); and alkanones, including nabumetone. For a moredetailed description of the NSAIDs, see Paul A. Insel, AnalgesicAntipyretic and Antiinflammatory Agents and Drugs Employed in theTreatment of Gout, in Goodman & Gilman's The Pharmacological Basis ofTherapeutics 617-57 (Perry B. Molinhoff and Raymond W. Ruddon eds., 9thed 1996) and Glen R. Hanson, Analgesic, Antipyretic and AntiInflammatory Drugs in Remington: The Science and Practice of PharmacyVol II 1196-1221 (A. R. Gennaro ed. 19th ed. 1995) which are herebyincorporated by reference in their entireties. Suitable Cox-IIinhibitors and 5-lipoxygenase inhibitors, as well as combinationsthereof, are described in U.S. Pat. No. 6,136,839, which is herebyincorporated by reference in its entirety. Examples of useful Cox IIinhibitors include, but are not limited to, rofecoxib and celecoxib.Examples of useful antimigraine agents include, but are not limited to,alpiropride, bromocriptine, dihydroergotamine, dolasetron, ergocomine,ergocominine, ergocryptine, ergonovine, ergot, ergotamine, flumedroxoneacetate, fonazine, ketanserin, lisuride, lomerizine, methylergonovine,methysergide, metoprolol, naratriptan, oxetorone, pizotyline,propranolol, risperidone, rizatriptan, sumatriptan, timolol, trazodone,zolmitriptan, and mixtures thereof.

Examples of useful β-adrenergic blockers include, but are not limitedto, acebutolol, alprenolol, amosulabol, arotinolol, atenolol, befunolol,betaxolol, bevantolol, bisoprolol, bopindolol, bucumolol, bufetolol,bufuralol, bunitrolol, bupranolol, butidrine hydrochloride, butofilolol,carazolol, carteolol, carvedilol, celiprolol, cetamolol, cloranolol,dilevalol, epanolol, esmolol, indenolol, labetalol, levobunolol,mepindolol, metipranolol, metoprolol, moprolol, nadolol, nadoxolol,nebivalol, nifenalol, nipradilol, oxprenolol, penbutolot, pindolol,practolol, pronethalol, propranolol, sotalol, sulfinalol, talinolol,tertatolol, tilisolol, timolol, toliprolol, and xibenolol.

Examples of useful anticonvulsants include, but are not limited to,acetylpheneturide, albutoin, aloxidone, aminoglutethimide,4-amino-3-hydroxybutyric acid, atrolactamide, beclamide, buramate,calcium bromide, carbamazepine, cinromide, clomethiazole, clonazepam,decimemide, diethadione, dimethadione, doxenitroin, eterobarb,ethadione, ethosuximide, ethotoin, felbamate, fluoresone, gabapentin,5-hydroxytryptophan, latnotrigine, magnesium bromide, magnesium sulfate,mephenytoin, mephobarbital, metharbital, methetoin, methsuximide,5-methyl-5-(3-phenanthryl)-hydantoin, 3-methyl-5-phenylhydantoin,narcobarbital, nimetazepam, nitrazepam, oxcarbazepine, paramethadione,phenacemide, phenetharbital, pheneturide, phenobarbital, phensuximide,phenylmethylbarbituric acid, phenytoin, phethenylate sodium, potassiumbromide, pregabaline, primidone, progabide, sodium bromide, solanum,strontium bromide, suclofenide, sulthiame, tetrantoin, tiagabine,topiramate, trimethadione, valproic acid, valpromide, vigabatrin, andzonisamide. Examples of useful antidepressants include, but are notlimited to, binedaline, caroxazone, citalopram, (S)-citalopram,dimethazan, fencamine, indalpine, indeloxazine hydrocholoride, nefopam,nomifensine, oxitriptan, oxypertine, paroxetine, sertraline, thiazesim,trazodone, benmoxine, iproclozide, iproniazid, isocarboxazid, nialamide,octamoxin, phenelzine, cotinine, rolicyprine, rolipram, maprotiline,metralindole, mianserin, mirtazepine, adinazolam, amitriptyline,amitriptylinoxide, amoxapine, butriptyline, clomipramine, demexiptiline,desipramine, dibenzepin, dimetacrine, dothiepin, doxepin, fluacizine,imipramine, imipramine N-oxide, iprindole, lofepramine, melitracen,metapramine, nortriptyline, noxiptilin, opipramol, pizotyline,propizepine, protriptyline, quinupramine, tianeptine, trimipramine,adrafinil, benactyzine, bupropion, butacetin, dioxadrol, duloxetine,etoperidone, febarbamate, femoxetine, fenpentadiol, fluoxetine,fluvoxamine, hematoporphyrin, hypericin, levophacetoperane,medifoxamine, milnacipran, minaprine, moclobemide, nefazodone,oxaflozane, piberaline, prolintane, pyrisuccideanol, ritanserin,roxindole, rubidium chloride, sulpiride, tandospirone, thozalinone,tofenacin, toloxatone, tranylcypromine, L-tryptophan, venlafaxine,viloxazine, and zimeldine.

Examples of useful anticancer agents include, but are not limited to,acivicin, aclarubicin, acodazole hydrochloride, acronine, adozelesin,aldesleukin, altretamine, ambomycin, ametantrone acetate,aminoglutethimide, amsacrine, anastrozole, anthramycin, asparaginase,asperlin, azacitidine, azetepa, azotomycin, batimastat, benzodepa,bicalutamide, bisantrene hydrochloride, bisnafide dimesylate, bizelesin,bleomycin sulfate, brequinar sodium, bropirimine, busulfan,cactinomycin, calusterone, caracemide, carbetimer, carboplatin,carmustine, carubicin hydrochloride, carzelesin, cedefingol,chlorambucil, cirolemycin, and cisplatin.

Therapeutic agents useful for treating or preventing an addictivedisorder include, but are not limited to, methadone, desipramine,arnantadine, fluoxetine, buprenorphine, an opiate agonist,3-phenoxypyridine, or a serotonin antagonist.

Examples of useful therapeutic agents for treating or preventingParkinson's disease and parkinsonism include, but are not limited to,carbidopa/levodopa, pergolide, bromocriptine, ropinirole, pramipexole,entacapone, tolcapone, selegiline, amantadine, and trihexyphenidylhydrochloride.

Examples of useful therapeutic agents for treating or preventing anxietyinclude, but are not limited to, benzodiazepines, such as alprazolam,brotizolam, chlordiazepoxide, clobazam, clonazepam, clorazepate,demoxepam, diazepam, estazolam, flumazenil, flurazepam, halazepam,lorazepam, midazolam, nitrazepam, nordazepam, oxazepam, prazepam,quazepam, temazepam, and triazolam; non-benzodiazepine agents, such asbuspirone, gepirone, ipsapirone, tiospirone, zolpicone, zolpidem, andzaleplon; tranquilizers, such as barbituates, e.g., amobarbital,aprobarbital, butabarbital, butalbital, mephobarbital, methohexital,pentobarbital, phenobarbital, secobarbital, and thiopental; andpropanediol carbamates, such as meprobamate and tybamate.

Examples of useful therapeutic agents for treating or preventingepilepsy or seizure include, but are not limited to, carbamazepine,ethosuximide, gabapentin, lamotrigine, phenobarbital, phenytoin,primidone, valproic acid, trimethadione, benzodiazepines, gamma-vinylGABA, acetazolamide, and felbamate.

Examples of useful therapeutic agents for treating or preventing strokeinclude, but are not limited to, anticoagulants such as heparin, agentsthat break up clots such as streptokinase or tissue plasminogenactivator, agents that reduce swelling such as mannitol orcorticosteroids, and acetylsalicylic acid.

Examples of useful therapeutic agents for treating or preventing apruritic condition include, but are not limited to, naltrexone;nalmefene; danazol; tricyclics such as amitriptyline, imipramine, anddoxepin; antidepressants such as those given below; menthol; camphor;phenol; pramoxine; capsaicin; tar; steroids; and antihistamines.

Examples of useful therapeutic agents for treating or preventingpsychosis include, but are not limited to, phenothiazines such aschlorpromazine hydrochloride, mesoridazine besylate, and thoridazinehydrochloride; thioxanthenes such as chloroprothixene and thiothixenehydrochloride; clozapine; risperidone; olanzapine; quetiapine;quetiapine fumarate; haloperidol; haloperidol decanoate; loxapinesuccinate; molindone hydrochloride; pimozide; and ziprasidone.

Examples of useful therapeutic agents for treating or preventing ALSinclude, but are not limited to, baclofen, neurotrophic factors,riluzole, tizanidine, benzodiazepines such as clonazepan and dantrolene.

Examples of useful therapeutic agents for treating or preventingcognitive disorders include, but are not limited to, agents for treatingor preventing dementia such as tacrine; donepezil; ibuprofen;antipsychotic drugs such as thioridazine and haloperidol; andantidepressant drugs such as those given below.

Examples of useful therapeutic agents for treating or preventing amigraine include, but are not limited to, sumatriptan; methysergide;ergotamine; caffeine; and beta-blockers such as propranolol, verapamil,and divalproex.

Examples of useful therapeutic agents for treating or preventingvomiting include, but are not limited to, 5-HT3 receptor antagonistssuch as odansetron, dolasetron, granisetron, and tropisetron; dopaninereceptor antagonists such as prochlorperazine, thiethylperazine,chlorpromazine, metoclopramide, and domperidone; glucocorticoids such asdexamethasone; and benzodiazepines such as lorazepam and alprazolam.

Examples of useful therapeutic agents for treating or preventingdyskinesia include, but are not limited to, reserpine and tetrabenazine.

Examples of useful therapeutic agents for treating or preventingdepression include, but are not limited to, tricyclic antidepressantssuch as amitryptyline, amoxapine, bupropion, clomipramine, desipramine,doxepin, imipramine, maprotiline, nefazadone, nortriptyline,protriptyline, trazodone, trimipramine, and venlafaxine; selectiveserotonin reuptake inhibitors such as citalopramn, (S)-citalopram,fluoxetine, fluvoxamine, paroxetine, and setraline; monoamine oxidaseinhibitors such as isocarboxazid, pargyline, phenelzine, andtranylcypromine; and psychostimulants such as dextroamphetamine andmethylphenidate.

A compound of the present invention and the second therapeutic agent canact additively or, in one embodiment, synergistically. In oneembodiment, a compound of the present invention is administeredconcurrently with the second therapeutic agent; for example, acomposition comprising an effective amount of a compound of Formula I,I′, I″, II or II′, and an effective amount of the second therapeuticagent can be administered. Alternatively, a composition comprising aneffective amount of a compound of Formula I, I′, I″, II or II′ and adifferent composition comprising an effective amount of the secondtherapeutic agent can be concurrently administered. In anotherembodiment, an effective amount of a compound of the present inventionis administered prior or subsequent to administration of an effectiveamount of the second therapeutic agent. In this embodiment, the compoundof the present invention is administered while the second therapeuticagent exerts its therapeutic effect, or the other therapeutic agent isadministered while the compound of the present invention exerts itspreventive or therapeutic effect for treating, ameliorating orpreventing a disorder or condition.

A pharmaceutical composition of the present invention can beadministered to any animal that may experience the beneficial effects ofa compound of the present invention. Foremost among such animals aremammals, e.g., humans and companion animals, although the invention isnot intended to be so limited.

A pharmaceutical composition of the present invention can beadministered by any means that achieves its intended purpose. Forexample, administration can be by the parenteral, subcutaneous,intravenous, intramuscular, intraperitoneal, transdermal, intranasal,rectal, intravaginal or buccal route, or by inhalation. Alternatively,or concurrently, administration can be by the oral route. The dosageadministered and route of administration will vary, depending upon thecircumstances of the particular subject, and taking into account suchfactors as age, health, and weight of the recipient, condition ordisorder to be treated, kind of concurrent treatment, if any, frequencyof treatment, and the nature of the effect desired.

A pharmaceutical composition of the present invention is preferablymanufactured in a manner which is itself known, for example, by means ofconventional mixing, granulating, dragee-making, dissolving, extrusion,or lyophilizing processes. Thus, pharmaceutical compositions for oraluse can be obtained by combining the active compound with solidexcipients, optionally grinding the resulting mixture and processing themixture of granules, after adding suitable auxiliaries, if desired ornecessary, to obtain tablets or dragee cores.

Suitable excipients include fillers such as saccharides (for example,lactose, sucrose, mannitol or sorbitol), cellulose preparations, calciumphosphates (for example, tricalcium phosphate or calcium hydrogenphosphate), as well as binders such as starch paste (using, for example,maize starch, wheat starch, rice starch, or potato starch), gelatin,tragacanth, methyl cellulose, hydroxypropylmethylcellulose, sodiumcarboxymethylcellulose, and/or polyvinyl pyrrolidone. If desired, one ormore disintegrating agents can be added, such as the above-mentionedstarches and also carboxymethyl-starch, cross-linked polyvinylpyrrolidone, agar, or alginic acid or a salt thereof, such as sodiumalginate.

Auxiliaries are typically flow-regulating agents and lubricants such as,for example, silica, talc, stearic acid or salts thereof (e.g.,magnesium stearate or calcium stearate), and polyethylene glycol. Drageecores are provided with suitable coatings that are resistant to gastricjuices. For this purpose, concentrated saccharide solutions may be used,which may optionally contain gum arabic, talc, polyvinyl pyrrolidone,polyethylene glycol and/or titanium dioxide, lacquer solutions andsuitable organic solvents or solvent mixtures. In order to producecoatings resistant to gastric juices, solutions of suitable cellulosepreparations such as acetylcellulose phthalate orhydroxypropymethyl-cellulose phthalate can be used. Dye stuffs orpigments may be added to the tablets or dragee coatings, for example,for identification or in order to characterize combinations of activecompound doses.

Examples of other pharmaceutical preparations that can be used orallyinclude push-fit capsules made of gelatin, or soft, sealed capsules madeof gelatin and a plasticizer such as glycerol or sorbitol. The push-fitcapsules can contain a compound in the form of granules, which may bemixed with fillers such as lactose, binders such as starches, and/orlubricants such as talc or magnesium stearate and, optionally,stabilizers, or in the form of extruded multiparticulates. In softcapsules, the active compounds are preferably dissolved or suspended insuitable liquids, such as fatty oils or liquid paraffin. In addition,stabilizers may be added.

Possible pharmaceutical preparations for rectal administration include,for example, suppositories, which consist of a combination of one ormore active compounds with a suppository base. Suitable suppositorybases include natural and synthetic triglycerides, and paraffinhydrocarbons, among others. It is also possible to use gelatin rectalcapsules consisting of a combination of active compound with a basematerial such as, for example, a liquid triglyceride, polyethyleneglycol, or paraffin hydrocarbon.

Suitable formulations for parenteral administration include aqueoussolutions of the active compound in a water-soluble form such as, forexample, a water-soluble salt, alkaline solution, or acidic solution.Alternatively, a suspension of the active compound may be prepared as anoily suspension. Suitable lipophilic solvents or vehicles for such assuspension may include fatty oils (for example, sesame oil), syntheticfatty acid esters (for example, ethyl oleate), triglycerides, or apolyethylene glycol such as polyethylene glycol-400 (PEG-400). Anaqueous suspension may contain one or more substances to increase theviscosity of the suspension, including, for example, sodiumcarboxymethyl cellulose, sorbitol, and/or dextran. The suspension mayoptionally contain stabilizers.

The following examples are illustrative, but not limiting, of thecompounds, compositions and methods of the present invention. Suitablemodifications and adaptations of the variety of conditions andparameters normally encountered in clinical therapy and which areobvious to those skilled in the art in view of this disclosure arewithin the spirit and scope of the invention.

In the following examples,

Examples Example A1 O-Pyridin-2-ylmethylhydroxylamine dihydrochloride

a) 2-Pyridiylmethanol (2.23 g, 20.0 mmol), N-hydroxyphthalimide (3.26 g,20.0 mmol) and triphenylphosphine (5.35 g, 20.0 mmol) were dissolved intetrahydrofuran (100 ml). Diethyl azodicarboxylate (40% in toluene, 10ml, 22.0 mmol) was added to this mixture, and stirred at roomtemperature for 3 hours. The solvent was evaporated under reducedpressure and the residue was suspended in ethanol (40 ml). The resultingprecipitate was collected and dried to give2-(pyridin-2-ylmethoxy)isoindole-1,3-dione (3.60 g, 71%).

b) 2-(Pyridin-2-ylmethoxy)isoindole-1,3-dione (2.03 g, 8.00 mmol) andhydrazine monohydrate (400 mg, 8.00 mmol) were dissolved in ethanol (15ml) and the mixture was refluxed for 1 hour. The solvent was evaporatedunder reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/methanol, 100/0-90/10) to giveO-pyridin-2-ylmethylhydroxylamine as pale yellow oil. The oil wasdissolved in ethyl acetate (15 ml) and methanol (10 ml), and then 4N—HClin ethyl acetate (20 ml) was added to this solution. The solvent wasevaporated under reduced pressure and the residue was suspended inhexane (30 ml). The resulting precipitate was collected and dried togive the title compound (1.37 g, 87%).

Example A2 O-(2-Chloropyridin-4-ylmethyl hydroxylamine

was prepared from (2-chloropyridin-4-yl)methanol as described in EXAMPLEA1.

Example A3 5-(Aminooxymethyl)-2-fluorobenzonitrile

was prepared from 2-fluoro-5-(hydroxymethyl)benzonitrile as described inEXAMPLE A1.

Example A4 O-((6-Methoxypyridin-2-yl)methyl)hydroxylamine

was prepared from (6-methoxypyridin-2-yl)methanol as described inEXAMPLE A1.

Example A5 O-((2-Methoxpyridin-3-yl)methyl)hydroxylamine

was prepared from (2-methoxypyridin-3-yl)methanol as described inEXAMPLE A1.

Example A6 O-((5-Fluoropyridin-2-yl)methyl)hydroxylamine

a) The mixture of 2-bromo-5-fluoropyridine (1.00 g, 0.5.68 mmol),palladium(II) acetate (127 mg, 0.568 mmol),1,1′-bis(diphenylphosphino)ferrocene (630 mg, 1.14 mmol) andtriethylamine (1.6 mmol) in ethano/N,N-dimethylformamide (1:1, 30 ml)was stirred under carbon monoxide atmosphere (1 atm) at 50° C. for 3hours. H2O (20 ml) was added and the whole was filtrated through a padof Celite. The filtrate was extracted with ethyl acetate, washed withH₂O and brine, dried (MgSO₄) and evaporated under reduced pressure. Theresidue was purified by column chromatography on silica (ethylacetate/hexane, 20/80-50/50) to give ethyl 5-fluoropicolinate (754 mg,78%, colorless solid).

b) To a solution of ethyl 5-fluoropicolinate (377 mg, 2.23 mmol).intetrahydrofuran (6 ml), LiBH₄ (73 mg, 3.34 mmol) was added at 0° C. andstirred at room temperature for 1 hour. The reaction was quenched withice-water and extracted with ethyl acetate, dried (Na₂SO₄) andevaporated under reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane, 20/80-60/40) to give(5-fluoropyridin-2-yl)methanol (309 mg, 54%, colorless oil).

c) O-((5-Fluoropyridin-2-yl)methyl)hydroxylamine was prepared from(5-fluoropyridin-2-yl)methanol as described in EXAMPLE A1.

Example A7 O-((3-Fluoropyridin-2-yl)methyl)hydroxylamine

was prepared from (3-fluoropyridin-2-yl)methanol as described in EXAMPLEA1.

Example A8 O-((5-Chloropyridin-2-yl)methyl)hydroxylamine

was prepared from (5-chloropyridin-2-yl)methanol as described in EXAMPLEA1.

Example A9 3-(Aminooxymethyl)-N,N-dimethylaniline

was prepared from (3-(dimethylamino)phenyl)methanol as described inEXAMPLE A1.

Example A10 O-((6-Methoxypyridin-3-yl)methyl)hydroxylamine

was prepared from (6-methoxypyridin-3-yl)methanol as described inEXAMPLE A1.

Example A11 O-((2-chloro-6-methoxypyridin-4-yl)methyl)hydroxylamine

was prepared from (2-chloro-6-methoxypyridin-4-yl)methanol as describedin EXAMPLE A1.

Example A12 O-((2-Methoxypyridin-4-yl)methyl)hydroxylamine

was prepared from (2-methoxypyridin-4-yl)methanol as described inEXAMPLE A1.

Example A13 (R)-tert-butyl 3-(aminooxymethyl)morpholine-4-carboxylate

was prepared from (S)-tert-butyl3-(hydroxymethyl)morpholine-4-carboxylate as described in EXAMPLE A1.

Example A14 (S)-tert-butyl 3-(aminooxymethyl)morpholine-4-carboxylate

was prepared from (R)-tert-butyl3-(hydroxymethyl)morpholine-4-carboxylate as described in EXAMPLE A1.

Example A15 2-(Aminooxymethyl)isonicotinonitrile

a) Sulfuric acid (1.5 ml) was added to the solution of 4-cyanopyridine(15.7 g, 151 mmol) in methanol (225 ml) at room temperature and refluxedfor 30 minutes. A solution of ammonium peroxodisulfate (54.9 g, 241mmol) in H₂O (100 ml) was slowly added over 30 minutes under reflux andthe mixture was refluxed with stirring for 1 hour. After cooling,precipitated materials were filtered off and methanol was removed fromthe filtrate under reduced pressure. The residue was neutralized (pH=9)by adding saturated aqueous K₂CO₃ solution and precipitated materialswere filtered off again. The filtrate was extracted with chloroform (100ml×4), dried (Na₂SO4) and evaporated under reduced pressure. The residuewas purified by column chromatography on silica (chloroform/methanol) togive 2-(hydroxymethyl)isonicotinonitrile (7.95 g, 39%, off-white solid).

b) 2-(aminooxymethyl)isonicotinonitrile was prepared from2-(hydroxymethyl)isonicotinonitrile as described in EXAMPLE A1.

Example A16 O-((4-Methoxypyridin-2-yl)methyl)hydroxylamine

was prepared from (4-methoxypyridin-2-yl)methanol as described inEXAMPLE A1.

Example A17 O-(Isoquinolin-1-yl)hydroxylamine

a) To a solution of potassium tert-butoxide (1.35 g, 12.0 mmol) inN,N-dimethylformamide (3 ml), a solution of ethyl acetohydroxamate (1.24g, 12.0 mmol) in N,N-dimethylformamide (3 ml) was added and stirred atroom temperature for 30 minutes. A solution of 1-chloroisoquinoline(1.72 g, 10.0 mmol) in N,N-dimethylformamide (4 ml) was added to thereaction mixture and stirred at room temperature for 2.5 hours.N,N-dimethylformamide was evaporated under reduced pressure and theresidue was diluted with ethyl acetate (200 ml), washed with H₂O (50ml), dried (MgSO4) and evaporated under reduced pressure. The residuewas purified by column chromatography on silica (ethyl acetate/hexane,20/80-40/60) to give (E)-ethyl N-isoquinolin-1-yloxyacetimidate (2.04 g,89%, pale-yellow oil).

b) To a solution of (E)-ethyl N-isoquinolin-1-yloxyacetimidate (2.00 g,8.68 mmol) in methanol/H₂O (3:1, 20 ml), sulfuric acid (1.85 ml) wasadded dropwise over 5 minutes and stirred at room temperature for 5hours. H₂O (30 ml) was added and neutralized (pH=9) by adding saturatedaqueous K₂CO₃ solution and precipitated materials were filtered off. Thefiltrate was diluted with ethyl acetate (100 ml), washed with H₂O (40ml) and brine, dried (MgSO4) and evaporated under reduced pressure. Theresidue was purified by column chromatography on silica (ethylacetate/hexane, 30/70) to give the title compound (607 mg, 32%,pale-yellow oil).

Example A18 3-(Aminooxy(cyclopropyl)methyl)benzonitrile

a) To a solution of 3-cyanobenzonitrile (1.33 g, 10.0 mmol) intetrahydrofuran (50 ml), cyclopropylmagnesium bromide (0.5 M solution intetrahydrofuran, 50 ml, 25 mmol) was added dropwise at −78° C. over 15minutes and stirred at −78° C. for 12 hours. The reaction was quenchedwith HCl (1 M, 50 ml), extracted with ethyl acetate, washed with brine,dried (MgSO₄) and evaporated under reduced pressure. The residue waspurified by column chromatography on silica (ethyl acetate/hexane,20/80-40/60) to give 3-(cyclopropyl(hydroxy)methyl)benzonitrile (1.08 g,60%, pale-yellow oil).

c) 3-(Aminooxy(cyclopropyl)methyl)benzonitrile was prepared from3-(cyclopropyl(hydroxy)methyl)benzonitrile as described in EXAMPLE A1.

Example A19 O-((4-Methoxyquinolin-2-yl)methyl)hydroxylamine

a) To a solution of 4-methoxy-2-quinolinecarboxylic acid (2.14 g, 10.0mmol) and K₂CO₃ (1.66 g, 12.0 mmol) in acetonitrile (40 ml) andN,N-dimethylformamide (50 ml), iodomethane (2.25 ml, 3.6 mmol) was addedand stirred at at 80° C. for 4 hours. The solvents were evaporated underreduced pressure and the residue was diluted with ethyl acetate (200ml), washed with H₂O (50 ml) and brine, dried (MgSO₄) and evaporatedunder reduced pressure. The residual solid was triturated with ethylacetate/hexane to give methyl 4-methoxyquinoline-2-carboxylate (1.57 g,72%, colorless solid).

b) O-((4-Methoxyquinolin-2-yl)methyl)hydroxylamine was prepared frommethyl 4-methoxyquinoline-2-carboxylate as described in EXAMPLE A6.

Example A20O-((4-Fluorophenyl)(6-methoxypyridin-3-yl)methyl)hydroxylamine

was prepared from 6-methoxynicotinaldehyde as described in EXAMPLE A18.

Example A213-(1-(Aminooxy)-2-(tert-butyldimethylsilyloxy)ethyl)benzonitrile

a) To a mixture of 3-acetylbenzonitrile (3.00 g, 20.4 mmol) and[bis(trifluoroacetoxy)iodo]benzene (17.6 g, 40.9 mmol) inacetonitrile/H₂O (5:1, 144 ml), trifluoroacetic acid (3.15 ml, 40.9mmol) was added and stirred at 80° C. for 10 hours. The solvent wasevaporated under reduced pressure and the residue was diluted with ethylacetate (120 ml), washed with saturated aqueous NaHCO3 solution (30 ml),dried (MgSO₄ and K₂CO₃) and evaporated under reduced pressure. Theresidue was purified by column chromatography on silica (ethylacetate/hexane, 45/55-65/35) to give 3-(2-hydroxyacetyl)benzonitrile(1.09 g, 33%, yellow solid).

b) To a solution of 3-(2-hydroxyacetyl)benzonitrile (1.08 g, 6.74 mmol)and imidazole (1.10 g, 16.2 mmol) in N,N-dimethylformamide (50 ml),tert-butylchlorodimethylsilyl chloride (2.10 g, 13.5 mmol) was added andstirred at 0° C. for 30 minutes. The solvent was evaporated underreduced pressure and the residue was diluted with ethyl acetate (120ml), washed with saturated aqueous NH₄Cl solution (30 ml) and brine,dried (MgSO₄) and evaporated under reduced pressure. The residue waspurified by column chromatography on silica (ethyl acetate/hexane,0/100-20/80) to give3-(2-(tert-butyldimethylsilyloxy)acetyl)benzonitrile (1.11 g, 60%,colorless oil).

c) To a solution of 3-(2-(tert-butyldimethylsilyloxy)acetyl)benzonitrile(1.10 g, 3.99 mmol) in methanol (20 ml), NaBH₄ (302 mg, 7.99 mmol) wasadded and stirred at 0° C. for 10 minutes. The solvent was evaporatedunder reduced pressure and the residue was diluted with ethyl acetate(100 ml), washed with saturated aqueous NaHCO₃ solution (30 ml) andbrine, dried (MgSO₄) and evaporated under reduced pressure. The residuewas purified by column chromatography on silica (ethyl acetate/hexane,5/95-30/70) to give3-(2-(tert-butyldimethylsilyloxy)-1-hydroxyethyl)benzonitrile (641 mg,58%, colorless oil).

d) 3-(1-(Aminooxy)-2-(tert-butyldimethylsilyloxy)ethyl)benzonitrile wasprepared from (4-methoxypyridin-2-yl)methanol as described in EXAMPLEA1.

Example A22 O-((5-Chlorobenzo[d]oxazol-2-yl)methyl)hydroxylamine

a) To a suspension of NaH (60%, 66 mg, 1.7 mmol) inN,N-dimethylfonnamide (5 ml), N-hydroxyphthalimide (269 mg, 1.65 mmol)and 5-chloro2-(chloromethyl)-1,3-benzoxazole (303 mg, 1.50 mmol) wasadded at 0° C. and stirred at 80° C. for 1 hour. The reaction wasquenched with H₂O (3 ml) and the precipitated material was collected,washed with H₂O and dried under reduced pressure at 80° C. to give2-((5-chlorobenzo[d]oxazol-2-yl)methoxy)isoindoline-1,3-dione.

b) A mixture of2-((5-chlorobenzo[d]oxazol-2-yl)methoxy)isoindoline-1,3-dione (295 mg,0.900 mmol) and hydrazine monohydrate (0.050 ml, 1 mmol) in ethanol (5ml) was stirred at room temperature for 3 hours. After cooling to 0° C.,precipitated materials were filtered off and the solvent was removedfrom the filtrate under reduced pressure to give the title compound (179mg, 100%, yellow solid).

Example A23 O-((1H-Indol-2-yl)methyl)hydroxylamine

was prepared from (1H-indol-2-yl)methanol as described in EXAMPLE A1.

Example A24O-((4-Fluorophenyl)(1-methyl-1H-imidazol-5-yl)methyl)hydroxylamine

a) To a solution of 1-methyl-1H-imidazole-5-carboxaldehyde (500 mg, 4.45mmol) in tetrahydrofuran (5 ml), 4-fluorophenylmagnesium bromide (1.0 Msolution in tetrahydrofuran, 6.20 ml, 6.20 mmol) was added dropwise at0° C. over 5 minutes and stirred at 0° C. for 30 minutes. The reactionwas quenched with saturated aqueous NH₄Cl solution (30 ml), extractedwith chloroform (50 ml×3), dried (MgSO₄) and evaporated under reducedpressure. The residue was purified by column chromatography on silica(ethyl acetate/methanol, 100/0-90/10) to give(4-fluorophenyl)(1-methyl-1H-imidazol-5-yl)methanol (443 mg, 48%,colorless solid).

b) To a solution of (4-fluorophenyl)(1-methyl-1H-imidazol-5-yl)methanol(270 mg, 1.31 mmol) in dichloromethane (10 ml), thionyl chloride (0.285ml, 3.93 mmol) was added dropwise at 0° C. and stirred at roomtemperature for 1 hour. The solvent was evaporated under reducedpressure and the crude product of5-(chloro(4-fluorophenyl)methyl)-1-methyl-1H-imidazole was used withoutfurther purification.

c) To a suspension of NaH (60%, 126 mg, 3.1 mmol) inN,N-dimethylformamide (8 ml), N-hydroxyphthalimide (256 mg, 1.57 mmol)was added at 0° C. and stirred at room temperature for 10 minutes. Asolution of crude product of5-(chloro(4-fluorophenyl)methyl)-1-methyl-1H-imidazole inN,N-dimethylformamide (7 ml) and KI (22 mg, 0.13 mmol) was added to thereaction mixture and stirred at 80° C. for 10 hours. The reaction wasquenched with H₂O (30 ml), extracted with ethyl acetate (50 ml×2),washed with brine, dried (MgSO₄) and evaporated under reduced pressure.The residue was purified by column chromatography on silica (ethylacetate/methanol, 100/0-90/10) to give2-((4-fluorophenyl)(1-methyl-1H-imidazol-5-yl)methoxy)isoindoline-1,3-dione(411 mg, 89%, pale-yellow solid).

d) To a solution of2-((4-fluorophenyl)(1-methyl-1H-imidazol-5-yl)methoxy)isoindoline-1,3-dione(200 mg, 0.569 mmol) in ethanol (2 ml), methylhydrazine (0.030 ml, 0.57mmol) was added and stirred at room temperature for 2 hours. Aftercooling to 0° C., precipitated materials were filtered off and thesolvent was removed from the filtrate under reduced pressure and thecrude product of title compound was used without further purification.

Example A25 tert-Butyl4-(aminooxy(4-fluorophenyl)methyl)piperidine-1-carboxylate

a) To a suspension of 4-(4-fluorobenzoyl)piperidine p-toluenesulfonate(2.00 g, 5.00 mmol) and triethylamine (0.840 ml, 6.00 mmol) indichloromethane (55 ml), a solution of di-t-butyldicarbonate (1.20 g,5.50 mmol) in dichloromethane (5 ml) was added and stirred at roomtemperature for 30 minutes. The reaction was quenched with saturatedaqueous NaHCO₃ solution (50 ml), extracted with chloroform (60 ml),dried (MgSO₄) and evaporated under reduced pressure. The residue waspurified by column chromatography on silica (ethyl acetate/hexane,5/95-30/70) to give tert-butyl4-(4-fluorobenzoyl)piperidine-1-carboxylate (1.56 g, 99%, colorlesssolid).

b) To a solution of tert-butyl4-(4-fluorobenzoyl)piperidine-1-carboxylate (1.55 g, 4.93 mmol) inmethanol (20 ml), NaBH₄ (302 mg, 7.99 mmol) was added and stirred atroom temperature for 1 hour. The solvent was evaporated under reducedpressure and the residue was diluted with ethyl acetate (100 ml), washedwith saturated aqueous NaHCO₃ solution (50 ml) and brine, dried (MgSO₄)and evaporated under reduced pressure to give tert-butyl4-((4-fluorophenyl)(hydroxy)methyl)piperidine-1-carboxylate (1.62 g,100%, colorless solid).

c) tert-butyl 4-(aminooxy(4-fluorophenyl)methyl)piperidine-1-carboxylatewas prepared from tert-butyl4-((4-fluorophenyl)(hydroxy)methyl)piperidine-1-carboxylate as describedin EXAMPLE A1.

Example A26 O-((1H-Indol-3-ylmethyl)hydroxylamine

a) To a suspension of NaH (60%, 88 mg, 2.2 mmol) inN,N-dimethylformnamide (6 ml), N-hydroxyphthalimide (359 mg, 2.20 mmol)was added at 0° C. and stirred at room temperature for 5 minutes.N-Boc-3-bromoindole (620 mg, 2.00 mmol) was added to the reactionmixture at 0° C. and stirred at 80° C. for 1 hour. The reaction wasquenched with H₂O, extracted with ethyl acetate, dried (MgSO₄) andevaporated under reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane, 10/90-50/50) to givetert-butyl3-((1,3-dioxoisoindolin-2-yloxy)methyl)-1H-indole-1-carboxylate (214 mg,27%, pale-red solid).

b) A mixture of tert-butyl3-((1,3-dioxoisoindolin-2-yloxy)methyl)-1H-indole-1-carboxylate (214 mg,0.550 mmol) and hydrazine monohydrate (0.032 ml, 0.65 mmol) in ethanol(3 ml) was stirred at room temperature for 1 hour. After cooling to 0°C., precipitated materials were filtered off and the solvent was removedfrom the filtrate under reduced pressure. The residue was purified bycolumn chromatography on silica (ethyl acetate/hexane, 20/80-50/50) togive tert-butyl 3-(aminooxymethyl)-1H-indole-1-carboxylate (86 mg, 60%,red oil).

c) To a solution of NaI (147 mg, 0.990 mmol) in acetonitrile (3 ml),chlorotrimethylsilane (0.130 ml, 0.990 mmol) was added and stirred atroom temperature for 15 minutes. A solution of tert-butyl3-(aminooxymethyl)-1H-indole-1-carboxylate (86 mg, 0.33 mmol) inacetonitrile (1 ml) was added to the reaction mixture and stirred at 60°C. for 1 hour. The reaction was quenched with H₂O and 10% aqueousNa₂S₂O₃ solution (3 ml), neutralized with ammonia solution, extractedwith ethyl acetate, dried (MgSO₄) and evaporated under reduced pressureand the crude product of title compound was used without furtherpurification.

Example A27 (S)-tert-Butyl 2-(aminooxymethyl)indoline-1-carboxylate

was prepared from (S)-tert-butyl 2-(hydroxymethyl)indoline-1-carboxylateas described in EXAMPLE A1.

Example A28 O-((1H-Benzo[d]imidazol-6-yl)methyl)hydroxylamine

a) To a solution of 1H-benzimidazole-5-carboxylic acid (4.87 g, 30.0mmol) in tetrahydrofuran (1 50 ml), LiAlH₄ (2.48 g, 60 mmol) was addedat −78° C. and stirred at room temperature overnight. The reaction wasquenched with methanol (5 ml) and H₂O (1 ml) at 0° C. and stirred atroom temperature for 1.5 hours. The precipitated materials were filteredoff and the filtrate was concentrated under reduced pressure. Theresidue was purified by column chromatography on silica(chloroform/methanol, 95/5-90/10) to give(1H-benzo[d]imidazol-6-yl)methanol (1.95 g, 44%, pale-yellow solid).

b) O-((1H-Benzo[d]imidazol-6-yl)methyl)hydroxylamine was prepared from(1H-benzo[d]imidazol-6-yl)methanol as described in EXAMPLE A1.

Example A29 O-(Benzo[d][1,3]dioxol-2-ylmethyl)hydroxylamine

a) To a mixture of pyrocatechol (2.20 g,20.0 mmol)-and sodium methoxide(2.16 g, 40.0 mmol) in methanol (25 ml), dichloroacetic acid methylester (2.10 ml, 20.0 mmol) was added and refluxed for 17 hours. Thereaction was quenched with HCl solution and the solvent was evaporatedunder reduced pressure. The residue was extracted with diethyl ether (50ml×2), dried (Na₂SO₄) and evaporated under reduced pressure. The residuewas purified by column chromatography on silica (ethyl acetate/hexane,0/100-50/50) to give methyl benzo[d][1,3]dioxole-2-carboxylate (744 mg,21%, colorless oil).

b) To a solution of methyl benzo[d][1,3]dioxole-2-carboxylate (735 mg,4.08 mmol) in tetrahydrofuran (30 ml), a suspension of LiAlH₄ (176 mg,4.49 mmol) in tetrahydrofuran (3 ml) was added at 0° C. and stirred atroom temperature for 1 hour. The reaction was quenched with saturatedaqueous NaHCO₃ solution (5 drops) and methanol (1 ml) at 0° C. andstirred at room temperature for 30 minutes. The precipitated materialswere filtered off and the filtrate was concentrated under reducedpressure to give benzo[d][1,3]dioxol-2-ylmethanol (432 mg, 71%,colorless oil).

c) O-(Benzo[d][1,3]dioxol-2-ylmethyl)hydroxylamine was prepared frombenzo[d][1,3]dioxol-2-ylmethanol as described in EXAMPLE A1.

Example A30 tert-Butyl2-(aminooxymethyl)-5-fluoro-1H-benzo[d]imidazole-1-carboxylate

a) A mixture of 4-fluoro-1,2-phenylenediamine (1.26 g, 10.0 mmol) andchloroacetic acid (1.23 g, 13.0 mmol) in HCl (6 M, 7 ml) was stirred at95° C. for 6 hours. The reaction mixture was neutralized with saturatedaqueous NaHCO₃ solution (pH=9) and the precipitated material wascollected, washed with H₂O and dried under reduced pressure at 65° C. togive 2-(chloromethyl)-5-fluoro-1H-benzo[d]imidazole (1.58 g, 86%,off-white solid).

b) To a solution of 2-(chloromethyl)-5-fluoro-1H-benzo[d]imidazole (921mg, 5.00 mmol) in 1,4-dioxane (20 ml), di-t-butyldicarbonate (3.50 ml,15.0 mmol) was added at room temperature and stirred at 90° C. for 6hours. The reaction was quenched with H₂O, extracted with ethyl acetate,dried (MgSO₄) and evaporated under reduced pressure. The residue waspurified by column chromatography on silica (ethyl acetate/hexane,10/90-90/10) to give tert-butyl2-(chloromethyl)-5-fluoro-1H-benzo[d]imidazole-1-carboxylate (982 mg,70%, pale-yellow oil).

c) tert-Butyl 2-(aminooxymethyl)-5-fluoro-1H-benzo[d]imidazole-1-carboxylate was prepared from tert-butyl2-(chloromethyl)-5-fluoro-1H-benzo[d]imidazole-1-carboxylate asdescribed in EXAMPLE A22.

Example A31 3-(Aminooxy(pyridin-4-yl)methyl)benzonitrile

a) To a solution of bis(2-dimethylaminoethyl) ether (1.13 ml, 6.00 mmol)in tetrahydrofuran (25 ml), isopropylmagnesium chloride (2.0 M intetrahydrofuran, 3.00 ml, 6.00 mmol) was added and stirred at roomtemperature for 30 minutes. To the reaction mixture, 3-iodobenzonitrile(1.14 g, 5.00 mmol) was added and stirred at room temperature for 10minutes, and 4-pyridinecarboxaldehyde (0.480 ml, 5.00 mmol) was addedand stirred at 0° C. for 1 hour. The reaction was quenched withsaturated aqueous NH₄Cl solution, extracted with ethyl acetate (50ml×3), dried (MgSO₄) and evaporated under reduced pressure. The residuewas purified by column chromatography on silica (ethyl acetate/methanol,100/0-80/20) to give 3-(hydroxy(pyridin-4-yl)methyl)benzonitrile (280mg, 27%, colorless solid).

b) 3-(Aminooxy(pyridin-4-yl)methyl)benzonitrile was prepared from3-(hydroxy(pyridin-4-yl)methyl)benzonitrile as described in EXAMPLE A24.

Example A32 3-(Aminooxy(pyridin-3-yl)methyl)benzonitrile

was prepared from nicotinaldehyde as described in EXAMPLE A31.

Example A33 3-(Aminooxy(pyridin-2-yl)methyl)benzonitrile

was prepared from picolinaldehyde as described in EXAMPLE A31.

Example A34 3-(1-(Aminooxy)-2-morpholinoethyl)benzonitrile

a) A solution of trimethylsulfonium iodide (4.49 g, 22.0 mmol) inacetonitrile (40 ml), KOH (2.64 g, 40.0 mmol) and H₂O (0.100 ml) wasadded at room temperature and stirred at 60° C. for 15 hours. Thereaction was quenched with brine, extracted with diethyl ether (100ml×2), washed with brine, dried (MgSO₄) and evaporated under reducedpressure. The residue was purified by column chromatography on silica(ethyl acetate/hexane, 25/75) to give 3-(oxiran-2-yl)benzonitrile (1.63g, 55%, colorless oil).

b) A solution of 3-(oxiran-2-yl)benzonitrile (650 mg, 4.47 mmol) inmorpholine (5 ml) was stirred at 80° C. for 20 hours. The solvent wasevaporated under reduced pressure and the residue was purified by columnchromatography on silica (chloroform/methanol, 97/3) to give3-(1-hydroxy-2-morpholinoethyl)benzonitrile (983 mg, 95%, colorlessoil).

c) 3-(1 -(Aminooxy)-2-morpholinoethyl)benzonitrile was prepared from3-(1-hydroxy-2-morpholinoethyl)benzonitrile as described in EXAMPLE A1.

Example A35 3-(1-(Aminooxy)-2-isopropoxyethyl)benzonitrile

a) NaH (60%, 240 mg, 6.00 mmol) was added to isopropanol (1 ml) andstirred at room temperature for 15 minutes. A solution of3-(oxiran-2-yl)benzonitrile (290 mg, 2.00 mmol) in isopropanol (4 ml)was added dropwise to the reaction mixture and refluxed for 8 hours. Thereaction was quenched with H₂O (10 ml) at 0° C., extracted with diethylether (30 ml×2), washed with brine, dried (MgSO₄) and evaporated underreduced pressure. The residue was purified by column chromatography onsilica (ethyl acetate/hexane, 30/70) to give3-(1-hydroxy-2-isopropoxyethyl)benzonitrile (100 mg, 24%, colorlessoil).

b) 3-(1-(Aminooxy)-2-isopropoxyethyl)benzonitrile was prepared from3-(1-hydroxy-2-isopropoxyethyl)benzonitrile as described in EXAMPLE A1.

Example A36 3-( 1 -(Aminooxy)-2-(4-fluorophenoxy)ethyl)benzonitrile

was prepared from 4-fluorophenol as described in EXAMPLE A35.

EXAMPLE A37 tert-Butyl2-(aminooxymethyl)-3H-imidazo[4,5-b]pyridine-3-carboxylate

a) After a mixture of 3,4-diaminopyridine (546 mg, 5.00 mmol) inpolyphosphoric acid (18 g) was heated at at 120° C. for 20 minutes,chloroacetonitrile (0.410 ml, 6.50 mmol) was added to the reactionmixture and heated under microwave irradiation at 200° C. for 30minutes. The reaction was quenched with H₂O (10 ml) at 0° C., pouredinto saturated aqueous NaHCO₃ solution, extracted with ethylacetate/methanol, dried (MgSO₄) and evaporated under reduced pressure.The residual solid was triturated with ethyl acetate/hexane (40:60) togive 2-(chloromethyl)-3H-imidazo[4,5-b]pyridine (510 mg, 61%, yellowsolid).

b) tert-Butyl 2-(aminooxymethyl)-3H-imidazo[4,5-b]pyridine-3-carboxylatewas prepared from 2-(chloromethyl)-3H-imidazo[4,5-b]pyridine asdescribed in EXAMPLE A30.

Example A38 O-(Cyclopropyl(4-fluorophenyl)methyl)hydroxylamine

was prepared from 4-fluorobenzaldehyde as described in EXAMPLE A18.

Example A39O-(Cyclopropyl(3-(trifluoromethyl)phenyl)methyl)hydroxylamine

was prepared from 3-trifluoromethylbenzaldehyde as described in EXAMPLEA18.

Example A40 tert-Butyl2-(aminooxymethyl)-6-chloro-3H-imidazo[4,5-b]pyridine-3-carboxylate

a) To a mixture of 2-amino-5-chloropyridine (2.57 g, 20.0 mmol) andsulfuric acid (6.30 ml), huming HNO₃ (0.860 ml, 21.1 mmol) was addeddropwise over 15 minutes at 55° C. and stirred at 55° C. for 1 hour.After cooling, the reaction mixture was poured into ice-water (60 g) andneutralized with aqueous NaOH solution (pH=11). The precipitatedmaterial was collected, washed with H₂O and dried under reduced pressureat 50° C. to give 5-chloro-3-nitropyridin-2-amine (2.31 g, 67%, yellowsolid).

b) To a suspension of 5-chloro-3-nitropyridin-2-amine (1.04 g, 6.00mmol) in ethanol (6 ml), SnCl₂.2H₂O (6.77 g, 30.0 mmol) was addedportionwise at room temperature and stirred at 90° C. for 1 hour. Aftercooling, the reaction mixture was basified with aqueous NaOH solution(pH=14), extracted with ethyl acetate, dried (MgSO₄) and evaporatedunder reduced pressure to give 5-chloropyridine-2,3-diamine (604 mg,70%, tan solid).

c) tert-Butyl2-(aminooxymethyl)-6-chloro-3H-imidazo[4,5-b]pyridine-3-carboxylate wasprepared from 5-chloropyridine-2,3-diamine as described in EXAMPLE A37.

Example A41 O-((3-Phenylpyridin-2-yl)methyl)hydroxylamine

a) A mixture of 3-hydroxypicolic acid (1.39 g, 10.0 mmol) and HCl (2 Min methanol, 60 ml) was refluxed for 6 hours. The solvent was removedunder reduced pressure and the residue was neutralized with saturatedaqueous NaHCO₃ solution, extracted with ethyl acetate, dried (MgSO₄) andevaporated under reduced pressure to give methyl 3-hydroxypicolinate(687 mg, 45%, colorless solid).

b) To a solution of 3-hydroxypicolinate (687 mg, 4.49 mmol) andtriethylamine (0.690 ml, 4.93 mmol) in dichloromethane (10 ml),trifluoromethanesulfonic anhydride (0.830 ml, 4.93 mmol) was addeddropwise at 0° C. and stirred at room temperature for 1 hour. Thereaction was quenched with H₂O, extracted with chloroform, dried (MgSO₄)and evaporated under reduced pressure. The residue was purified bycolumn chromatography on silica (ethyl acetate/hexane, 20/80-50/50) togive methyl 3-(trifluoromethylsulfonyloxy)picolinate (1.22 g, 95%,pale-yellow oil).

c) A mixture of methyl 3-(trifluoromethylsulfonyloxy)picolinate (610 mg,2.14 mmol), phenylboronic acid (274 mg, 2.25 mmol),tetrakis(triphenylphosphine)palladium (74 mg, 0.064 mmol) and K₂CO₃ (591mg, 4.28 mmol) in toluene (10 ml) was stirred at 90° C. for 1 hour.After cooling, the reaction was quenched with H₂O, extracted with ethylacetate, dried (MgSO₄) and evaporated under reduced pressure. Theresidue was purified by column chromatography on silica (ethylacetate/hexane, 30/70-50/50) to give methyl 3-phenylpicolinate (467 mg,100%, yellow oil).

d) To a solution of methyl 3-phenylpicolinate (467 mg, 2.19 mmol).intetrahydrofuran (5 ml), LiBH₄ (72 mg, 3.3 mmol) was added at 0° C. andstirred at room temperature for 1.5 hours. The reaction was quenchedwith H₂O and extracted with ethyl acetate, dried (MgSO₄) and evaporatedunder reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane, 30/70-50/50) to give(3-phenylpyridin-2-yl)methanol (186 mg, 46%, yellow oil).

e) O-((3-Phenylpyridin-2-yl)methyl)hydroxylamine was prepared from(3-phenylpyridin-2-yl)methanol as described in EXAMPLE A1.

Example A42 O-((2-Chloropyridin-3-yl)methyl)hydroxylamine

was prepared from (2-chloropyridin-3-yl)methanol as described in EXAMPLEA1.

Example A43 O-((3-Chloropyridin-4-yl)methyl)hydroxylamine

was prepared from 3-chloro-4-(chloromethyl)pyridine as described inEXAMPLE A22.

Example A44 O-((6-Chloropyridin-2-yl)methyl)hydroxylamine

was prepared from 2-chloro-6-(chloromethyl)pyridine as described inEXAMPLE A22.

Example A45 O-((4-Chloropyridin-3-yl)methyl)hydroxylamine

was prepared from 4-chloro-3-(chloromethyl)pyridine as described inEXAMPLE A22.

Example A46 O-((2-Chloropyridin-4-yl)methyl)hydroxylamine

was prepared from 2-chloro-4-(chloromethyl)pyridine as described inEXAMPLE A22.

Example A47 O-((3-Chloropyridin-2-yl)methyl)hydroxylamine

was prepared from 3-chloropyridine as described in EXAMPLE A15.

Example A48 5-(Aminooxymethyl)nicotinonitrile

was prepared from 5-(chloromethyl)nicotinonitrile as described inEXAMPLE A22.

Example 1 1-((S)-4-Methyl-2-methylaminopentanoyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

a) 4-Piperidone monohydrate hydrochloride (1.10 g, 7.00 mmol) andN-Boc-N-methylleucine (1.89 g, 7.70 mmol) were suspended inN,N-dimethylformamide (70 ml). 1-Hydroxybenzotriazole (946 mg, 7.00mmol), N-ethyldimethylaminopropylcarbodiimide hydrochloride (1.61 g,8.40 mmol) and triethylamine (1.17 ml, 8.40 mmol) were added to thesuspension, and the mixture was stirred at 60° C. for 8 hours. Thesolvent was evaporated under reduced pressure. The residue was dilutedwith ethyl acetate (50 ml), poured into saturated aqueous NaHCO3solution (50 ml) and extracted with ethyl acetate (100 ml×2). Theorganic layer was washed with brine, dried (MgSO₄) and evaporated underreduced pressure. The residue was purified by column chromatography onsilica (ethyl acetate/hexane, 40/60-60/40) to give[(S)-1-(4,4-dihydroxypiperidine-1-carbonyl)-3-methylbutyl]methylcarbamicacid tert-butyl ester (2.28 g, 94%, pale yellow solid).

b)[(S)-1-(4,4-Dihydroxypiperidine-1-carbonyl)-3-methylbutyl]methylcarbamicacid tert-butyl ester (172 mg, 0.50 mmol),O-(3-trifluoromethylbenzyl)hydroxylamine hydrochloride (114 mg, 0.50mmol) and sodium acetate (41 mg, 0.50 mmol) were suspended in ethanol (5ml). The mixture was stirred at room temperature for 1 hour. The solventwas evaporated under reduced pressure, the residue was diluted withethyl acetate (20 ml), washed with H₂O (5 ml), dried (MgSO₄) andevaporated under reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane, 20/80-50/50) to give[(S)-1-(4-benzyloxyiminopiperidine-1-carbonyl)-3-methylbutyl]methylcarbamicacid tert-butyl ester (250 mg, 98%, colorless oil).

c)[(S)-1-(4-Benzyloxyiminopiperidine-1-carbonyl)-3-methylbutyl]methylcarbamicacid tert-butyl ester (250 mg, 0.50 mmol) was dissolve in ethyl acetate(2.5 ml) and cooled to 0° C. The mixture was added 4N—HCl in ethylacetate (2.5 ml) and stirred at room temperature for 8 hours. Thesolvent was removed under reduced pressure. The residue was trituratedwith ether (10 ml) to give the title compound (170 mg, 80%).

Example 2 1-((S)-4-Methyl-2-methylaminopentanoyl)piperidin-4-oneO-benzyloxime hydrochloride

was prepared as described in EXAMPLE 1

Example 3 1-((S)-4-Methyl-2-methylaminopentanoyl)piperidin-4-oneO-(4-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 1

Example 4 1-((S)-4-Methyl-2-methylaminopentanoyl)piperidin-4-oneO-(4-chlorobenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 1.

¹H—NMR (DMSO-d₆) δ: 9.02 (1H, brs), 7.41 (2H, d), 7.39 (2H, d), 5.01(2H, s), 4.52-4.40 (1H, m), 3.92-3.68 (2H, m), 3.58-3.38 (2H, m),2.80-2.36 (7H, m), 1.80-1.52 (3H, m), 0.98-0.82 (6H, m).

Example 5 1-((S)-4-Methyl-2-methylaminopentanoyl)piperidin-4-oneO-pyridin-4-ylmethyloxime oxalate

was prepared as described in EXAMPLE 1. The free base was dissolved inether and oxalic acid (2.0 eq) was added to the solution. The resultingprecipitate was collected and dried in vacuo to give the title compound.

Example 6 1-((S)-4-Methyl-2-methylaminopentanoyl)piperidin-4-oneO-pyridin-2-ylmethyl-oxime oxalate

was prepared as described in EXAMPLE 1. Starting material wasO-pyridin-2-ylmethylhydroxylamine dihydrochloride (see example A1). Thefree base was dissolved in ether and oxalic acid (2.0 eq) was added tothe solution. The resulting precipitate was filtrated and dried in vacuoto give the title compound.

Example 7 1-((S)-4-Methyl-2-methylaminopentanoyl)piperidin-4-oneO-(2-chloropyridin-4-ylmethyl)oxime oxalate

was prepared as described in EXAMPLE 1. Starting material wasO-(2-chloropyridin-4-ylmethyl)hydroxylamine (see example A2).

Example 8 1-((S)-2-Amino-4-methylpentanoyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 1. BOC group was deprotected byusing trifluoroacetic acid.

¹H—NMR (DMSO-d₆) δ: 8.32 (1H, s), 7.71-7.57 (4H, m), 5.18 (2H, s),4.41-4.38 (1H, m), 3.78-3.74 (2H, m), 3.50-3.23 (2H, m), 2.81-2.31 (4H,m), 1.85-1.62 (3H, m), 0.97-0.93 (6H, m).

Example 9 1-((S)-4-Methyl-2-methylaminopentanoyl)piperidin-4-oneO-(3-chlorobenzyl)oxime hydrochloride

a)[(S)-1-(4,4-Dihydroxypiperidine-1-carbonyl)-3-methylbutyl]methylcarbamicacid tert-butyl ester (517 mg, 1.50 mmol), hydroxylamine hydrochloride(125 mg, 1.80 mmol) and sodium acetate (150 mg, 1.80 mmol) weresuspended in ethanol (15 ml). The mixture was stirred at roomtemperature for 2 hours. The solvent was evaporated under reducedpressure. The residue was diluted with ethyl acetate (50 ml), washedwith H₂O (20 ml), dried (MgSO₄) and evaporated under reduced pressure togive[(S)-1-(4-hydroxyiminopiperidine-1-carbonyl)-3-methylbutyl]methylcarbamicacid tert-butyl ester (512 mg, 100%, colorless solid).

b)[(S)-1-(4-Hydroxyiminopiperidine-1-carbonyl)-3-methylbutyl]methylcarbamicacid tert-butyl ester (125 mg, 0.365 mmol) and 3-chlorobenzyl bromide(83 mg, 0.402 mmol) was dissolved in N,N-dimethylformamide (5 ml). Thesolution was cooled to 0° C. and NaH (31 mg, 2.1 mmol) was added to themixture under nitrogen atmosphere. The mixture was stirred at 0° C. for1 hour and at room temperature for 30 minutes. The reaction was quenchedwith H₂O (15 ml) and extracted with ethyl acetate (30 ml×2). The organiclayer was washed with brine, dried (MgSO₄) and evaporated under reducedpressure. The residue was purified by column chromatography on silica(ethyl acetate/hexane, 20/80-40/60) to give{(S)-1-[4-(3-chlorobenzyloxyimino)piperidine-1-carbonyl]-3-methylbutyl}methylcarbamicacid tert-butyl ester (139 mg, 82%, colorless oil).

c){(S)-1-[4-(3-Chlorobenzyloxyimino)piperidine-1-carbonyl]-3-methylbutyl}methylcarbamicacid tert-butyl ester (135 mg, 0.290 mmol) was dissolve in ethyl acetate(1 ml) and cooled to 0° C. The mixture was added 4N—HCl in ethyl acetate(2 ml) and stirred at room temperature for 6 hours. The solvent wasremoved under reduced pressure and the resulting precipitate wasrecrystallized from ethyl acetate/methanol to give the title compound(74 mg, 63%).

Example 103-[1-((S)-4-Methyl-2-methylaminopentanoyl)piperidin-4-ylideneaminooxymethyl]benzonitrilehydrochloride

was prepared as described in EXAMPLE 9

Example 11 1-((S)-4-Methyl-2-methylaminopentanoyl)piperidin-4-oneO-(2-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 9

Example 12 1-[4,4-Bis-(4-fluorophenyl)butyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime oxalate

a) 1,4-Dioxa-8-azaspiro[4.5]decane (1.43 g, 10.0 mmol), and1,1′-(4-chlorobutylidene)-bis(4-fluorobenzene) (3.43 g, 11.0 mmol) wasdissolved in acetonitrile (100 ml). KI (332 mg, 2.0 mmol) and K₂CO₃(3.32 g, 24.0 mmol), was added to the solution, and the mixture wasrefluxed for 2 days. The solvent was removed under reduced pressure. H₂O(50 ml), was added to the residue, extracted with chloroform (80 ml×2),dried (MgSO₄) and evaporated under reduced pressure. The residue waspurified by column chromatography on silica (ethyl acetate/methanol,100/0-90/10) to give8-[4,4-bis-(4-fluorophenyl)butyl]-1,4-dioxa-8-azaspiro[4.5]decane (3.45g, 89%, colorless oil).

b) To a solution of8-[4,4-Bis-(4-fluorophenyl)butyl]-1,4-dioxa-8-azaspiro[4.5]decane (3.09g, 7.98 mmol) in tetrahydrofuran (50 ml), 2N—HClaq. (16 ml) was addedand refluxed for 24 hours. The mixture was neutralized with 2N—NaOHaq.at 0° C. and extracted with ethyl acetate (50 ml×2). The organic layerwas washed with brine, dried (MgSO₄) and evaporated under reducedpressure. The residue was purified by column chromatography on silica(ethyl acetate/methanol, 100/0-90/10) to give1-[4,4-bis-(4-fluorophenyl)butyl]piperidine-4,4-diol (2.41 g, 84%, paleyellow oil).

c) 1-[4,4-Bis-(4-fluorophenyl)butyl]piperidine-4,4-diol (289 mg, 0.80mmol), O-(3-trifluoromethylbenzyl)hydroxylamine hydrochloride (182 mg,0.80 mmol) and sodium acetate (66 mg, 0.80 mmol) were suspended inethanol (5 ml). The mixture was stirred at room temperature for 1 hour.The solvent was evaporated under reduced pressure. The residue wasdiluted with ethyl acetate (20 ml), washed with H₂O (5 ml), dried(MgSO₄) and evaporated under reduced pressure. The residue was purifiedby column chromatography on silica (ethyl acetate/hexane, 30/70-60/40)to give 1-[4,4-bis-(4-fluorophenyl)butyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (398 mg, 96%, colorless oil). To asolution of this free base in ethanol (2 ml), a solution of oxalic acid(79 mg, 0.85 mmol) in ethanol (1 ml) was added. The resultingprecipitate was collected and dried to give the title compound.

¹H—NMR (DMSO-d₆) δ: 7.73-7.57 (4H, m), 7.35-7.29 (4H, m), 7.15-7.07 (4H,m), 5.12 (2H, s), 4.09-4.00 (1H, m), 2.99-2.88 (6H, m), 2.71-2.67 (2H,m), 2.41-2.38 (2H, m), 2.05-1.91 (2H, m), 1.48-1.44 (2H, m).

Example 13 1-[4,4-Bis-(4-fluorophenyl)butyl]piperidin-4-oneO-(4-chlorobenzyl)oxime oxalate

was prepared as described in EXAMPLE 12

Example 14 1-[4,4-Bis-(4-fluorophenyl)butyl]piperidin-4-oneO-phenyloxime oxalate

was prepared as described in EXAMPLE 12

Example 15 1-[4,4-Bis-(4-fluorophenyl)butyl]piperidin-4-oneO-phenethyloxime oxalate

was prepared as described in EXAMPLE 12

Example 16 1-[4,4-Bis-(4-fluorophenyl)butyl]piperidin-4-oneO-pyridin-3-ylmethyloxime dioxalate

was prepared as described in EXAMPLE 12

¹H—NMR (DMSO-d₆) δ: 8.56 (1H, d), 8.52 (1H, dd), 7.76 (1H, dt), 7.39(1H, dd), 7.33 (4H, dd), 7.11 (4H, t), 5.08 (2H, s), 4.03-3.98 (1H, m),3.34-3.10 (6H, m), 2.76-2.72 (2H, m), 2.05-1.91 (2H, m), 1.53-1.50 (2H,m).

Example 17 1-[4,4-Bis-(4-fluorophenal)butyl]piperidin-4-oneO-pyridin-4-ylmethyloxime dioxalate

was prepared as described in EXAMPLE 12

Example 18 1-[4,4-Bis-(4-fluorophenyl)butyryl]piperidin-4-oneO-pyridin-3-ylmethyloxime oxalate

a) 4-Piperidone monohydrate hydrochloride (313 mg, 2.00 mmol) and4,4-bis-(4-fluorophenyl)butyric acid (608 mg, 2.20 mmol) were suspendedin N,N-dimethylformamide (20 ml). 1-Hydroxybenzotriazole (270 mg, 2.00mmol), N-ethyldimethylaminopropylcarbodiimide hydrochloride (460 mg,2.40 mmol) and triethylamine (0.225 ml, 2.40 mmol) were added to thesuspension and the mixture was stirred at 50° C. for 8 hours. Thesolvent was evaporated under reduced pressure. The residue was dilutedwith chloroform (10 ml), poured into saturated aqueous NaHCO₃ solution(30 ml), extracted with chloroform (100 ml×2), dried (MgSO₄) andevaporated under reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane, 50/50-70/30) to give1-(4,4-dihydroxypiperidin-1-yl)-4,4-bis-(4-fluorophenyl)butan-1-one (668mg, 89%, pale yellow oil).

b) 1-(4,4-Dihydroxypiperidin-1-yl)-4,4-bis-(4-fluorophenyl)butan-1-one(300 mg, 0.80 mmol), O-pyridin-3-ylmethylhydroxylamine dihydrochloride(158 mg, 0.80 mmol) and sodium acetate (131 mg, 1.60 mmol) weresuspended in ethanol (8 ml). The mixture was stirred at room temperaturefor 2 hours. The solvent was evaporated under reduced pressure. Theresidue was diluted with ethyl acetate (30 ml), washed with H₂O (10 ml),dried (MgSO₄) and evaporated under reduced pressure. The residue waspurified by column chromatography on silica (ethyl acetate/methanol,100/0-90/10) to give 1-[4,4-bis-(4-fluorophenyl)butyryl]piperidin-4-oneO-pyridin-3-ylmethyloxime (307 mg, 83%, pale yellow oil). To a solutionof this free base in ether (5 ml), oxalic acid (62 mg, 0.664 mmol) inether (2 ml) was added. The resulting precipitate was collected anddried to give the title compound.

¹H—NMR (DMSO-d₆) δ: 8.60-8.46 (2H, m), 7.76 (1H, d), 7.40 (1H, dd),7.38-7.23 (4H, dd), 7.08 (4H, t), 5.02 (2H, s), 4.04-3.98 (1H, m),3.58-3.28 (4H, m), 2.51-2.41 (2H, m), 2.31-2.08 (6H, m).

Example 19 1-[4,4-Bis-(4-fluorophenyl)butyryl]piperidin-4-oneO-pyridin-4-ylmethyloxime oxalate

was prepared as described in EXAMPLE 18

¹H—NMR (DMSO-d₆) δ: 8.55-8.50 (2H, m), 7.34-7.32 (6H, m), 7.12-7.09 (4H,m), 5.10 (2H, s), 4.00 (1H, t), 3.16-3.08 (6H, m), 2.83-2.80 (2H, m),2.51-2.49 (2H, m), 2.03-2.01 (2H, m), 1.55-1.52 (2H, m)

Example 20 1-Benzoylpiperidin-4-one O-(3-trifluoromethylbenzyl)oxime

Piperidin-4-one O-(3-trifluoromethylbenzyl)oxime (218 mg, 0.80 mmol) andbenzoic acid (107 mg, 0.88 mmol) were dissolved in dichloromethane (4ml). 1-Hydroxybenzotriazole (108 mg, 0.80 mmol) andN-ethyldimethylaminopropylcarbodiimide hydrochloride (184 mg, 0.96 mmol)were added to the mixture and stirred at room temperature for 1 hour.Saturated aqueous NaHCO₃ solution (10 ml) was added, extracted withchloroform (30 ml×2), dried (MgSO₄) and evaporated under reducedpressure. The residue was purified by column chromatography on silica(ethyl acetate/hexane, 20/80-40/60) to give the title compound (193 mg,64%).

Example 211-Phenyl-2-[4-(3-trifluoromethylbenzyloxyimino)piperidin-1-yl]ethane-1,2-dione

was prepared as described in EXAMPLE 20

Example 222-Oxo-N-phenyl-2-[4-(3-trifluoromethylbenzyloxyimino)piperidin-1-yl]acetamide

was prepared as described in EXAMPLE 20

Example 23 4-(3-Trifluoromethylbenzyloxyimino)piperidine-1-carboxylicacid phenylamide

To a solution of piperidin-4-one O-(3-trifluoromethylbenzyl)oxime (218mg, 0.80 mmol) in acetonitrile (2 ml), a solution of phenylisocyanate(114 mg, 0.96 mmol) in acetonitrile (2 ml) was added. The mixture andstirred at room temperature for 30 minutes. Methanol (10 ml) was addedand evaporated under reduced pressure. The residue was purified bycolumn chromatography on silica (ethyl acetate/hexane, 10/80-40/60) togive the title compound (178 mg, 57%).

Example 24 1-((S)-3-Amino-5-methylhexanoyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime oxalate

a) 1-Boc-4-piperidone (2.03 g, 10.0 mmol),O-(3-trifluoromethylbenzyl)hydroxylamine hydrochloride (2.28 g, 10.0mmol) and sodium acetate (820 mg, 10.0 mmol) were suspended in ethanol(100 ml). The mixture was stirred at room temperature for 3 hours. Thesolvent was evaporated under reduced pressure. The residue was dilutedwith ethyl acetate (100 ml), washed with H₂O (30 ml), dried (MgSO₄) andevaporated under reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane, 5/95-25/75) to give4-(3-trifluoromethylbenzyloxyimino)piperidine-1-carboxylic acidtert-butyl ester (3.15 g, 85%, colorless oil).

b) To a solution of4-(3-trifluoromethylbenzyloxyimino)piperidine-1-carboxylic acidtert-butyl ester (3.14 g, 8.34 mmol) in ethyl acetate (30 ml), 4N—HCl inethyl acetate (30 ml) was added at 0° C. and stirred at room temperaturefor 2 hours. The solvent was removed under reduced pressure to givepiperidin-4-one O-(3-trifluoromethylbenzyl)oxime hydrochloride (2.57 g,100%, pale yellow solid).

c) To a solution of piperidin-4-one O-(3-trifluoromethylbenzyl)oximehydrochloride (247 mg, 0.80 mmol) and N-Boc-L-β-homoleucine (216 mg,0.88 mmol) in dichloromethane (4 ml), 1-hydroxybenzotriazole (108 mg,0.80 mmol), N-ethyldimethylaminopropylcarbodiimide hydrochloride (184mg, 0.96 mmol) and triethylamine (0.135 ml, 0.96 mmol) was added andstirred at room temperature for 2 hours. Saturated aqueous NaHCO₃solution (10 ml) was added, extracted with chloroform (20 ml×2), dried(MgSO₄) and evaporated under reduced pressure. The residue was purifiedby column chromatography on silica (ethyl acetate/hexane, 35/65-60/40)to give((S)-3-methyl-1-{2-oxo-2-[4-(3-trifluoromethylbenzyloxyimino)piperidin-1-yl]ethyl}butyl)carbamicacid tert-butyl ester (340 mg, 85%, colorless oil).

d) To a solution of((S)-3-Methyl-1-{2-oxo-2-[4-(3-trifluoromethylbenzyloxyimino)piperidin-1-yl]ethyl}butyl)carbamicacid tert-butyl ester (340 mg, 0.646 mmol) in chloroform (8 ml),trifluoroacetic acid (4 ml) was added at 0° C. and stirred at roomtemperature for 2 hours. The solvent was removed under reduced pressure.Saturated aqueous NaHCO₃ solution (10 ml) was added and extracted withethyl acetate (30 ml×2). The organic layer was washed with brine, dried(MgSO₄) and evaporated under reduced pressure. The residue was purifiedby column chromatography on silica (chloroform/methanol, 95/5-85/15) togive 1-((S)-3-amino-5-methylhexanoyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (243 mg, 90%, pale yellow oil). To asolution of this free base in ethanol (3 ml), oxalic acid (55 mg, 0.608mmol) in ethanol (1 ml) was added. The solvent was removed under reducedpressure to give the title compound.

¹H—NMR (DMSO-d₆) δ: 7.66-7.57 (4H, m), 5.13 (2H, s), 3.57-3.45 (3H, m),2.78-2.28 (6H, m), 1.76-1.67 (1H, m), 1.40 (2H, dt), 0.87 (6H, t).

Example 25 1-((S)-2-Amino-3-phenylpropionyl)piperidin-4-oneO-(3-trifluoromethylbenzyloxime oxalate

was prepared as described in EXAMPLE 24

Example 26 1-((S)-2-Amino-4-methylpentanoyl)piperidin-4-oneO-benzyloxime hydrochloride

was prepared as described in EXAMPLE 24. Boc group was deprotected byusing 4N—HCl in ethyl acetate.

Example 27 1-((S)-3-Amino-5-methylhexanoyl)piperidin-4-one O-benzyloximehydrochloride

was prepared as described in EXAMPLE 24. Boc group was deprotected byusing 4N—HCl in ethyl acetate.

Example 28 1-((S)-2-Amino-3-phenylpropionyl)piperidin-4-oneO-benzyloxime hydrochloride

was prepared as described in EXAMPLE 24. Boc group was deprotected byusing 4N—HCl in ethyl acetate.

Example 29 1-[4,4-Bis-(4-fluorophenyl)butyryl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

Piperidin-4-one O-(3-trifluoromethylbenzyl)oxime hydrochloride (247 mg,0.80 mmol) and 4,4-bis-(4-fluorophenyl)butyric acid (243 mg, 0.88 mmol)were dissolved in dichloromethane (4 ml). 1-Hydroxybenzotriazole (108mg, 0.80 mmol), N-ethyldimethylaminopropylcarbodiimide hydrochloride(184 mg, 0.96 mmol) and triethylamine (0.135 ml, 0.96 mmol) were addedto the mixture and stirred at room temperature for 1 hour. Saturatedaqueous NaHCO₃ solution (10 ml) was added, extracted with chloroform (20ml×2), dried (MgSO₄) and evaporated under reduced pressure. The residuewas purified by column chromatography on silica (ethyl acetate/hexane,35/65-60/40) to give the title compound (420 mg, 99%).

¹H—NMR (DMSO-d₆) δ: 7.72-7.58 (4H, m), 7.38-7.24 (4H, m), 7.18-7.02 (4H,m), 5.10 (2H, s), 4.04-3.98 (1H, m), 3.60-3.30 (4H, m), 2.54-2.42 (2H,m), 2.30-2.18 (6H, m).

Example 30 1-[4,4-Bis-(4-fluorophenyl)butyryl]piperidin-4-oneO-(4-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 29

¹H-NMR (DMSO-d₆) δ: 7.63 (4H, dd), 7.21 (8H, dt), 5.13 (2H, s), 4.03(1H, s), 3.44 (6H, t), 2.51 (3H, s), 2.24 (6H, s).

Example 31 1-[4,4-Bis-(4-fluorophenyl)butyryl]piperidin-4-oneO-benzyloxime

was prepared as described in EXAMPLE 29

¹H-NMR (DMSO-d₆) δ: 7.57 (6H, dd), 5.03 (1H, s), 3.49 (5H, dd),2.73-2.31 (6H, m), 1.76 (1H, t), 1.48 (2H, dt), 0.87 (6H, t).

Example 32 1-[4,4-Bis-(4-fluorophenyl)butyl]piperidin-4-oneO-benzyloxime oxalate

Piperidin-4-one O-benzyloxime hydrochloride (100 mg, 0.49 mmol) and1,1′-(4-chlorobutylidene)-bis-(4-fluorobenzene) (144 mg, 0.51 mmol) wasdissolved in N,N-dimethylformamide (3 ml). KI (8 mg, 0.05 mmol) andK₂CO₃ (203 mg, 1.47 mmol) were added to the mixture and heated forovernight. After quenching with H₂O (3 ml), the mixture was extractedwith ethyl acetate (30 ml×3), washed with brine (×2), dried over Na₂SO₄and evaporated under reduced pressure. The residue was purified bycolumn chromatography on silica (ethyl acetate/hexane, 1/9-2/3) to givethe desired compound as the pale yellow oil. To a solution of this freebase in ethanol (1 ml), a solution of oxalic acid (23 mg, 0.255 mmol) inethanol (1 ml) was added. The resulting white precipitate was collected,washed with diethyl ether (2 ml) and dried under reduced pressure at 70°C. to give the title compound.

Example 33 1-[4,4-Bis-(4-fluorophenyl)butyl]piperidin-4-oneO-(4-trifluoromethylbenzyl)oxime oxalate

was prepared as described in EXAMPLE 32

Example 34 1-(3-Isobutylaminopropionyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

a) To a solution of piperidin-4-one O-(3-trifluoromethylbenzyl)oximehydrochloride (946 mg, 3.63 mmol) and acryl chloride (0.315 ml, 3.88mmol) in dichloromethane was added pyridine (0.313 ml, 3.88 mmol) at 0°C. and stirred at room temperature for 30 min. After quenching with H₂O(3 ml), the mixture was extracted by chloroform/H₂O (×3), dried overNa₂SO₄ and concentrated in vacuo. The residue was purified by columnchromatography on silica (ethyl acetate/hexane, 1/3-4/1) to give1-but-3-enoylpiperidin-4-one O-(3-trifluoromethylbenzyl)oxime (500 mg,42%, colorless oil).

b) 1-But-3-enoylpiperidin-4-one O-(3-trifluoromethylbenzyl)oxime (80 mg,0.25 mmol), isobutylamine (0.248 ml, 2.5 mmol) and ethanol (1.5 ml) weremixed together in a sealed tube and heated at 150° C. with microwaveequipment for 30 min. The reaction mixture was evaporated in vacuo andthe residue was purified by column chromatography on silica gel(chloroform/methanol/NH₃aq.=100/10/1) to afford the desired compound asa free base, which was dissolved in ethyl acetate (2 ml) and treatedwith 4N—HCl in ethyl acetate (2 ml) solution. The resulting mixture wasconcentrated in vacuo and dried under reduced pressure for 24 hours at70° C. to afford the title compound.

Example 35 1-[3-(4-Hydroxypiperidin-1-yl)propionyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 34

Example 36 1-[3-(4-Hydroxycyclohexylamino)propionyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 34

Example 37 1-[3-(2-Hydroxyethylamino)propionyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 34

Example 38 1-[3-(3-Hydroxypropylamino)propionyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 34

Example 39 1-{3-[(2-Hydroxyethyl)methylamino]propionyl}piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 34

Example 40 1-[3-(2-Morpholin-4-ylethylamino)propionyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 34

Example 41 1-(3-Morpholin-4-ylpropionyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 34

Example 421-[3-(4-Hydroxy-4-phenylpiperidin-1-yl)propionyl]-piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 34

Example 43 1-[3-(4-Methylpiperazin-1-yl)propionyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime dihydrochloride

was prepared as described in EXAMPLE 34

Example 44 1-[3-(4-Phenylpiperazin-1-yl)propionyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime dihydrochloride

was prepared as described in EXAMPLE 34

Example 45 1-[3-(4-Acetylpiperazin-1-yl)propionyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 34

Example 461-{3-[4-(2-Hydroxyethyl)piperazin-1-yl]propionyl}piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime dihydrochloride

was prepared as described in EXAMPLE 34

Example 47 1-[3-(4-Phenylpiperidin-1-ylpropionyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 34

¹H-NMR (DMSO-d₆) δ: 11.00 (1H, s), 7.68-7.60 (4H, m), 7.29 (5H, d), 5.15(2H, s), 3.59 (6H, t), 3.12-3.03 (4H, m), 2.86-1.92 (10H, m).

Example 48 1-[3-(4-Benzylpiperidin-1-yl)propionyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 34

¹H-NMR (DMSO-d₆) δ: 10.60 (1H, s), 7.64 (4H, dd), 7.25 (5H, d), 5.14(2H, s), 3.56-3.20 (12H, m), 2.97-2.29 (10H, m), 1.96-1.56 (5H, m).

Example 49 1-(2-Morpholin-4-ylethanesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

a) To a solution of piperidin-4-one O-(3-trifluoromethylbenzyl)oxime(100 mg, 0.37 mmol) in dichloromethane (5 ml), 2-chloroethansulfonylchloride (120 mg, 0.74 mmol) and triethylamine (0.103 ml, 0.74 mmol) indichloromethane (3 ml) was slowly added to this mixture at 0° C. andstirred for 15 minutes. Saturated aqueous NaHCO₃ solution (10 ml) wasadded, extracted with chloroform (20 ml×2), dried (MgSO₄) and evaporatedunder reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane, 25/75-50/50) to afford1-ethenesulfonylpiperidin-4-one O-(3-trifluoromethylbenzyl)oxime (106mg, 80%, colorless oil).

b) 1-Ethenesulfonyl-piperidin-4-one O-(3-trifluoromethyl-benzyl)-oxime(93 mg, 0.27 mmol) was dissolved in ethanol (1 ml). Morpholine (0.112ml, 1.28 mmol) was added to this mixture and stirred at room temperaturefor 12 hours. The reaction mixture was concentrated under reducedpressure. Then residue was diluted with ethyl acetate (30 ml), washedwith H₂O and brine. The organic layer was dried over MgSO₄ andconcentrated to dryness to afford the title compound (120 mg, 100%).

Example 50 1-(4-Butyl-benzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

To a solution of piperidin-4-one O-(3-trifluoromethylbenzyl)oximehydrochloride (247 mg, 0.80 mmol) and triethylamine (0.246 ml, 1.76mmol) in dichloromethane (4 ml), a solution of 4-butylbenzenesulfonylchloride (243 mg, 0.88 mmol) in dichloromethane (1 ml) was slowly addedat 0° C. and stirred at room temperature for 30 minutes. Saturatedaqueous NaHCO₃ solution (10 ml) was added, extracted with chloroform (20ml×2), dried (MgSO₄) and evaporated under reduced pressure. The residuewas purified by column chromatography on silica (ethyl acetate/hexane,10/90-40/60) to give the title compound (345 mg, 92%).

¹H-NMR (DMSO-d₆) δ: 7.62-7.49 (8H, m), 5.07 (2H, s), 3.06-2.99 (4H, m),2.68-2.63 (4H, m), 2.32 (2H, t), 1.63-1.53 (2H, m), 1.33-1.28 (2H, m),0.90 (3H, t).

Example 51 1-Benzenesulfonylpiperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

¹H-NMR (DMSO-d₆) δ: 7.80-7.50 (9H, m), 5.08 (2H, s), 3.12-3.00 (4H, m),2.64 (2H, t), 2.31 (2H, t).

Example 52 1-Methanesulfonylpiperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

Example 534-[4-(3-Trifluoromethylbenzyloxyimino)piperidine-1-sulfonyl]benzonitrile

was prepared as described in EXAMPLE 50

¹H-NMR (DMSO-d₆) δ: 8.18 (2H, d), 7.97 (2H, d), 7.70-7.56 (4H, m), 5.08(2H, s), 3.20-3.06 (4H, m), 2.63 (2H, t), 2.36 (2H, t).

Example 54 1-(1-Methyl-1H-imidazole-4-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

Example 55 1-(4-Trifluoromethylbenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

Example 56 1-(3-Trifluoromethylbenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

¹H-NMR (DMSO-d₆) δ: 8.18-8.06 (2H, m), 7.99 (1H, s), 7.90 (1H, t),7.64-7.52 (4H, m), 5.06 (2H, s), 3.20-3.08 (4H, m), 2.64 (2H, t), 2.34(2H, t).

Example 57 1-(2-Trifluoromethylbenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

Example 58 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

¹H-NMR (DMSO-d₆) δ: 7.92 (2H, d), 7.70-7.52 (6H, m), 5.04 (2H, s),3.14-3.02 (4H, m), 2.64 (2H, t), 2.32 (2H, t).

Example 59 1-(3-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

¹H-NMR (DMSO-d₆) δ: 7.84-7.78 (3H, m), 7.72 (1H, s), 7.68-7.56 (4H, m),5.08 (2H, s), 3.18-3.06 (4H, m), 2.62 (2H, t), 2.34 (2H, t).

Example 60 1-(2-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

Example 61 1-(4-Methoxybenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

Example 62 1-(4-Fluorobenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

¹H-NMR (DMSO-d₆) δ: 7.92-7.80 (2H, m), 7.72-7.42 (6H, m), 5.06 (2H, s),3.16-2.98 (4H, m), 2.63 (2H, t), 2.32 (2H, t).

Example 63 1-(2-Fluorobenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 50

¹H-NMR (DMSO-d₆) δ: 7.82-7.68 (2H, m), 7.64-7.38 (6H, m), 5.06 (2H, s),3.28-3.16 (4H, m), 2.62 (2H, t), 2.33 (2H, t).

Example 64 1-(6-Chloropyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

To a solution of piperidin-4-one O-(3-trifluoromethylbenzyl)oxime (1.09g, 4.0 mmol) and triethylamine (1.23 ml, 8.8 mmol) in dichloromethane(15 ml), 6-chloropyridine-3-sulfonyl chloride (933 mg, 4.4 mmol) indichloromethane (5 ml) was slowly added at 0° C. and stirred for 30minutes. Saturated aqueous NaHCO₃ solution (15 ml) was added, extractedwith chloroform (50 ml×2), dried (MgSO₄) and evaporated under reducedpressure. The residue was purified by column chromatography on silica(ethyl acetate/hexane, 20/80-45/55) to afford the title compound (1.75g, 98%).

¹H-NMR (DMSO-d₆) δ: 8.78 (1H, d), 8.21 (1H, dd), 7.80 (1H, d), 7.68-7.50(4H, m), 5.04 (2H, s), 3.22-3.04 (4H, m), 2.63 (2H, t), 2.36 (2H, t).

Example 65 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-(3-chlorobenzyl)oxime

a) To a suspension of 4-piperidone monohydrate hydrochloride (1.10 g,7.00 mmol) in dichloromethane (50 ml), N,N-diisopropylethylamine (7.71ml, 45.0 mmol) and a solution of p-butylbenzenesulfonyl chloride (3.49g, 15.0 mmol) in dichloromethane (25 ml) were added, and the mixture wasstirred at room temperature for 7 hours. Saturated aqueous NaHCO₃solution (20 ml) was added, extracted with chloroform (50 ml×2), dried(MgSO₄) and evaporated under reduced pressure. The residue was purifiedby column chromatography on silica (ethyl acetate/hexane, 25/75-45/55)to afford 1-(4-butylbenzenesulfonyl)piperidine-4,4-diol (3.88 g, 83%,yellow solid).

b) A suspension of 1-(4-butyl-benzenesulfonyl)piperidine-4,4-diol (1.57g, 5.0 mmol), hydroxyammonium chloride (417 mg, 6.0 mmol) and sodiumacetate (492 mg, 6.0 mmol) in ethanol (20 ml) was stirred at roomtemperature for 2 hours. The reaction mixture was concentrated underreduced pressure. Saturated aqueous NaHCO₃ solution (25 ml) was added,extracted with ethyl acetate (80 ml×2), washed with brine dried (MgSO₄)and evaporated under reduced pressure. The residue was recrystallizedfrom ethyl acetate/hexane to give1-(4-butylbenzenesulfonyl)piperidin-4-one oxime (1.02 g, 66%, colorlesssolid).

c) To a solution of 1-(4-butylbenzenesulfonyl)piperidin-4-one oxime (94mg, 0.30 mmol) and 3-chlorobenzyl bromide (74 mg, 0.36 mmol) intetrahydrofuran (4 ml), NaH was added under nitrogen atmosphere andstirred at 60° C. for 1 hour. The reaction was quenched with H₂O (5 ml),extracted with ethyl acetate (20 ml×2), washed with brine, dried (MgSO₄)and evaporated under reduced pressure. The residue was purified bycolumn chromatography on silica (ethyl acetate/hexane, 20/80-40/60) toafford the title compound (120 mg, 92%).

¹H-NMR (DMSO-d₆) δ: 7.63 (2H, d), 7.48 (2H, d), 7.38-7.20 (4H, m), 4.98(2H, s), 3.12-2.98 (4H, m), 2.72-2.59 (4H, m), 2.32 (2H, t), 1.58 (2H,quintet), 1.32 (2H, dt), 0.90 (3H, t).

Example 66 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-(4-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 65

Example 67 1-(4-Butylbenzenesulfonyl)piperidin-4-one O-benzyloxime

was prepared as described in EXAMPLE 65

¹H-NMR (DMSO-d₆) δ: 7.65 (2H, d), 7.37 (7H, t), 4.96 (2H, s), 3.03 (4H,d), 2.67 (2H, s), 2.50 (1H, s), 2.31 (2H, s), 1.56 (2H, s), 1.29 (2H,d), 0.88 (3H, s).

Example 68 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-pyridin-2-ylmethyloxime

was prepared as described in EXAMPLE 65

¹H-NMR (DMSO-d₆) δ: 8.44 (1H, dd), 7.72 (1H, dt), 7.63 (2H, d), 7.42(2H, d), 7.30-7.21 (2H, m), 5.02 (2H, s), 3.10-3.01 (4H, m), 2.73-2.60(4H, m), 2.31 (2H, t), 1.56 (2H, quintet), 1.28 (2H, dt), 0.90 (3H, t).

Example 69 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-(2-chloropyridin-4-ylmethyl)oxime

was prepared as described in EXAMPLE 65.

¹H-NMR (DMSO-d₆) δ: 8.36 (1H, d), 7.68 (2H, d), 7.46 (2H, d), 7.34 (1H,s), 7.28 (1H, d), 5.02 (2H, s), 3.11-3.01 (4H, m), 2.78-2.60 (4H, m),2.28-2.23 (2H, m), 1.56 (2H, quintet), 1.30 (2H, dt), 0.90 (3H, t).

Example 70 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-pyridin-3-ylmethyloxime

was prepared as described in EXAMPLE 65.

¹H-NMR (DMSO-d₆) δ: 8.60-8.42 (2H, m), 7.81-7.61 (3H, m), 7.59-7.30 (3H,m), 5.03 (2H, s), 3.18-2.94 (4H, m), 2.76-2.50 (4H, m), 2.40-2.28 (2H,m), 1.58 (2H, quintet), 1.31 (2H, dt), 0.90 (3H, t).

Example 71 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-pyridin-4-ylmethyloxime

was prepared as described in EXAMPLE 65.

¹H-NMR (DMSO-d₆) δ: 8.50 (2H, d), 7.68 (2H, d), 7.48 (2H, d), 7.23 (2H,d), 5.03 (2H, s), 3.13-3.01 (4H, m), 2.76-2.62 (4H, m), 2.38-2.24 (2H,m), 1.59 (2H, quintet), 1.32 (2H, dt), 0.92 (3H, t).

Example 72 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-(4-chlorobenzyl)oxime

was prepared as described in EXAMPLE 65.

¹H-NMR (DMSO-d₆) δ: 7.64 (2H, d), 7.48 (2H, d), 7.38 (2H, d), 7.30 (2H,d), 4.98 (2H, s), 3.12-2.98 (4H, m), 2.74-2.58 (4H, m), 2.32 (2H, t),1.58 (2H, quintet), 1.31 (2H, dt), 0.92 (3H, t).

Example 73 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-(4-chloropyridin-2-ylmethyl)oxime

was prepared as described in EXAMPLE 65.

¹H-NMR (DMSO-d₆) δ: 8.51 (1H, d), 7.68 (2H, d), 7.52-7.40 (3H, m), 7.36(1H, s), 5.03 (2H, s), 3.13-3.01 (4H, m), 2.74-2.62 (4H, m), 2.34 (2H,t), 1.58 (2H, quintet), 1.32 (2H, dt), 0.91 (3H, t).

Example 74 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-[1-(3-trifluoromethylphenyl)ethyl]oxime

was prepared as described in EXAMPLE 65.

¹H-NMR (DMSO-d₆) δ: 7.70-7.41 (8H, m), 5.21 (1H, q), 3.22-3.02 (2H, m),2.92-2.80 (2H, m), 2.79-2.54 (4H, m), 2.37-2.19 (2H, m), 1.58 (2H,quintet), 1.41 (3H, d), 1.36 (2H, dt), 0.90 (3H, t).

Example 75 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-(6-chloropyridin-2-ylmethyl)oxime

was prepared as described in EXAMPLE 65

¹H-NMR (DMSO-d₆) δ: 7.82 (1H, t), 7.68 (2H, d), 7.48 (2H, d), 7.39 (1H,d), 7.31 (1H, d), 5.00 (2H, s), 3.12-3.02 (4H, m), 2.70-2.62 (4H, m),2.32 (2H, t), 1.58 (2H, quintet), 1.30 (2H, dt), 0.90 (3H, t).

Example 76 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-(6-methoxypyridin-2-ylmethyl)oxime

was prepared as described in EXAMPLE 65.

¹H-NMR (DMSO-d₆) δ: 7.68 (2H, d), 7.61 (2H, d), 7.48 (2H, d), 6.88 (1H,d), 6.63 (1H, d), 4.98 (2H, s), 3.80 (3H, s), 3.12-3.02 (4H, m),2.73-2.63 (4H, m), 2.34 (2H, t), 1.58 (2H, quintet), 1.32 (2H, dt), 0.91(3H, t).

Example 773-[1-(4-Butylbenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]benzonitrile

was prepared as described in EXAMPLE 65

¹H-NMR (DMSO-d₆) δ: 7.78-7.42 (8H, m), 5.01 (2H, s), 3.12-2.98 (4H, m),2.72-2.58 (4H, m), 2.33 (2H, t), 1.58 (2H, quintet), 1.32 (2H, dt), 0.88(3H, t).

Example 78 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-(2-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 65.

¹H-NMR (DMSO-d₆) δ: 7.78-7.42 (8H, m), 5.13 (2H, s), 3.12-3.00 (4H, m),2.74-2.60 (4H, m), 2.32 (2H, t), 1.58 (2H, quintet), 1.31 (2H, dt), 0.89(3H, t).

Example 79 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethoxybenzyl)oxime

was prepared as described in EXAMPLE 65

¹H-NMR (DMSO-d₆) δ: 7.64 (2H, d), 7.50-7.40 (3H, m), 7.38-7.20 (3H, m),5.02 (2H, s), 3.12-2.98 (4H, m), 2.72-2.60 (4H, m), 2.32 (2H, t), 1.58(2H, quintet), 1.32 (2H, dt), 0.92 (3H, t).

Example 80 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-(3-methoxybenzyl)oxime

was prepared as described in EXAMPLE 65

¹H-NMR (DMSO-d₆) δ: 7.68 (2H, d), 7.42 (2H, d), 7.22 (1H, t), 6.90-6.80(3H, m), 4.96 (2H, s), 3.72 (3H, s), 3.12-2.98 (4H, m), 2.72-2.58 (4H,m), 2.32 (2H, t), 1.58 (2H, quintet), 1.32 (2H, dt), 0.90 (3H, t).

Example 81 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-(4-fluoro-3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 65.

¹H-NMR (DMSO-d₆) δ: 7.72-7.62 (4H, m), 7.50-7.42 (3H, m), 5.02 (2H, s),3.10-2.98 (4H, m), 2.72-2.58 (4H, m), 2.32 (2H, t), 1.58 (2H, quintet),1.30 (2H, dt), 0.90 (3H, t).

Example 82 1-(4-Butylbenzenesulfonyl)piperidin-4-oneO-cyclohexylmethyloxime

was prepared as described in EXAMPLE 65

¹H-NMR (DMSO-d₆) δ: 7.62 (2H, d), 7.42 (2H, d), 3.68 (2H, d), 3.10-2.92(4H, m), 2.62 (2H, t), 2.50 (2H, t), 2.18 (2H, t), 1.70-1.43 (8H, m),1.38-1.00 (5H, m), 0.96-0.78 (5H, m).

Example 83 1-(4-Aminobenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

a) To a solution of 4-piperidone monohydrate hydrochloride (2.38 g, 15.0mmol) in pyridine (15 ml) and dichloromethane (5 ml),4-nitrobenzenesulfonyl chloride (3.49 g, 16.5 mmol) in dichloromethane(10 ml) was slowly added at 0° C. and stirred at room temperature for2.5 hours. The solvent was evaporated under reduced pressure and theresidue was diluted with ethyl acetate (10 ml). HCl (1 M, 50 ml) wasadded, extracted with chloroform (100 ml×2), dried (MgSO₄) andevaporated under reduced pressure. The residue was purified by columnchromatography on silica (chloroform/methanol, 100/0-90/20) andrecrystallized from ethyl acetate/hexane to give1-(4-nitrobenzenesulfonyl)piperidine-4,4-diol (1.83 g, 40%, pale yellowsolid).

b) A suspension of 1-(4-nitrobenzenesulfonyl)piperidine-4,4-diol (351mg, 1.16 mmol), O-(3-trifluoromethylbenzyl)hydroxylamine hydrochloride(264 mg, 1.16 mmol) and sodium acetate (95 mg, 1.16 mmol) in ethanol (12ml) was stirred at room temperature for 1 hour. The solvent wasevaporated under reduced pressure. Saturated aqueous NaHCO₃ solution (10ml) was added, extracted with chloroform (30 ml×2), dried (MgSO₄) andevaporated under reduced pressure to give1-(4-nitrobenzenesulfonyl)piperidine-4-oneO-(3-trifluoromethylbenzyl)oxime (530 mg, 100%, colorless solid).

c) 1-(4-Nitrobenzenesulfonyl)piperidine-4-oneO-(3-trifluoromethylbenzyl)oxime (530 mg, 1.16 mmol) was taken up intoluene (10 ml). To the mixture, Fe (324 mg, 5.8 mmol), NH₄Cl (620 mg,11.6 mmol) and H₂O (1 ml) was added. The reaction mixture was heated at115° C. and stirred for 3 hours. The reaction mixture was diluted with30 ml of ethyl acetate, then filtrated through a pad of Celite. Thefiltrate was concentrated under reduced pressure. The residue waspurified by column chromatography on silica (ethyl acetate/hexane,30/70-50/50) to afford 1-(4-aminobenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (471 mg, 95%, pale yellow oil). To asolution of the free base in ethyl acetate, 4N—HCl in ethyl acetate wasadded. The resulting precipitate was collected and dried in vacuo togive the title compound.

Example 84 1-(3-Aminobenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 83

Example 85 1-(2-Aminobenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 83

¹H-NMR (DMSO-d₆) δ: 7.68-7.50 (4H, m), 7.41 (1H, d), 7.32 (1H, t), 6.86(1H, d), 6.62 (1H, t), 6.08 (2H, s), 5.10 (2H, s), 3.22-3.10 (4H, m),2.60 (2H, t), 2.28 (2H, t).

Example 86 1-[4-(2-Hydroxyethylamino)benzenesulfonyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

1-(4-Aminobenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (145 mg, 0.34 mmol) and pyridine (35mg, 0.45 mmol) was taken up in 1 ml of chloroform. Chloroformic acid2-chloroethyl ester (49 mg, 0.34 mmol) in chloroform (1 ml) was addedover 5 minutes, and stirred at room temperature for 10 minutes. Thesolvent was evaporated under reduced pressure. The residue was dissolvein ethanol (6 ml) and H₂O (2 ml). To the mixture, KOH (152 mg, 2.72mmol) was added. The mixture was heated at 100° C. and stirred for 15hours. The reaction mixture was concentrated under reduced pressure. Theresidue was dissolved in ethyl acetate (40 ml) and the mixture waswashed with H₂O and brine. The organic layer was dried over MgSO₄ andconcentrated in vacuo. The residue was purified by column chromatographyon silica (ethyl acetate/methanol, 100/0-90/10) to afford1-[4-(2-hydroxyethylamino)benzenesulfonyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (112 mg, 70%, colorless oil). To asolution of the free base in ethyl acetate (1 ml), 4N—HCl in ethylacetate (1 ml) was added. The solvent was removed under reducedpressure. The residue was triturated with ether (10 ml) to give thetitle compound.

Example 87 1-[3-(2-Hydroxyethylamino)benzenesulfonyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 86

Example 88 1-[2-(2-Hydroxyethylamino)benzenesulfonyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride

was prepared as described in EXAMPLE 86

Example 892-Amino-N-{4-[4-(3-trifluoromethylbenzyloxyimino)piperidine-1-sulfonyl]phenyl}acetamidehydrochloride

a) To a solution of 1-(4-aminobenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime hydrochloride (125 mg, 0.29 mmol) andBoc-glycine (61 mg, 0.35 mmol) in dichloromethane (5 ml),1-hydroxybenzotriazole (40 mg, 0.29 mmol) andN-ethyldimethylaminopropylcarbodiimide hydrochloride (167 mg, 0.35 mmol)were added and stirred at room temperature for 36 hours. Saturatedaqueous NaHCO₃ solution (10 ml) was added, extracted with chloroform (20ml×2), dried (MgSO₄) and evaporated under reduced pressure. The residuewas purified by column chromatography on silica (ethyl acetate/hexane,35/65-70/30) to give({4-[4-(3-trifluoromethylbenzyloxyimino)piperidine-1-sulfonyl]phenylcarbamoyl}methyl)carbamicacid tert-butyl ester (147 mg, 83%, colorless solid).

b) To a solution of({4-[4-(3-trifluoromethylbenzyloxyimino)piperidine-1-sulfonyl]phenylcarbamoyl}methyl)carbamicacid tert-butyl ester (147 mg, 0.24 mmol) in ethyl acetate (2 ml),4N—HCl in ethyl acetate (2 ml) was added at 0° C. and stirred at roomtemperature for 1.5 hours. The mixture was diluted with ether (30 ml)and precipitate was collected and dried to give the title compound (124mg, 99%).

Example 90 1-[4-(2-Aminoethylamino)benzenesulfonyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime dihydrochloride

1-(4-Fluorobenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (100 mg, 0.23 mmol) and ethylenediamine(70 mg, 1.16 mmol) were dissolved in toluene and stirred at 110° C. for12 hours. The reaction mixture was diluted with 30 ml of ethyl acetateand washed with H₂O and brine. The organic layer was dried over MgSO₄and concentrated. The residue was purified by column chromatography onsilica (ethyl acetate/methanol, 100/0-90/10) to afford the desiredcompound as a free base (65 mg, 60%), which was dissolved in dioxane (2ml) and treated with 4N—HCl in dioxane (2 ml) solution. The mixture wastriturated with ether (10 ml) to give the title compound.

Example 91 1-(4-Ethoxybenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

Under nitrogen atmosphere, sodium (27 mg, 1.16 mmol) was added toethanol (1 ml) and stirred at room temperature for 1 hour. A solution of1-(4-fluorobenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (100 mg, 0.23 mmol) in tetrahydrofuran(1 ml) was added to this mixture and refluxed for 4 hours. The reactionmixture was concentrated under reduced pressure. Saturated aqueous NH4Clsolution (5 ml) was added, extracted with ethyl acetate (20 ml×2),washed with brine, dried (MgSO₄) and evaporated under reduced pressure.The residue was purified by column chromatography on silica (ethylacetate/hexane, 20/80-40/60) to afford the title compound.

¹H-NMR (DMSO-d₆) δ: 7.72-7.52 (6H, m), 7.12 (2H, d), 5.04 (2H, s), 4.13(2H, q), 3.08-2.92 (4H, m), 2.62 (2H, t), 2.32 (2H, t), 1.37 (3H, t).

Example 92 1-(4-Propoxybenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 91

Example 93 1-(4-Isopropoxybenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 91

¹H-NMR (DMSO-d₆) δ: 7.70-7.56 (6H, m), 7.10 (2H, d), 5.04 (2H, s),4.80-4.64 (1H, m), 3.04-2.92 (4H, m), 2.62 (2H, t), 2.32 (2H, t), 1.32(6H, d).

Example 94 1-[4-(2-Methoxyethoxy)benzenesulfonyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 91

¹H-NMR (DMSO-d₆) δ: 7.72-7.51 (6H, m), 7.16 (2H, d), 5.07 (2H, s), 4.19(2H, t), 3.68 (2H, t), 3.32 (3H, s), 3.10-2.94 (4H, m), 2.62 (2H, t),2.32 (2H, t).

Example 95 1-(4-Cyclopropylmethoxybenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 91

¹H-NMR (DMSO-d₆) δ: 7.72-7.50 (6H, m), 7.10 (2H, d), 5.03 (2H, s), 3.91(2H, d), 3.04-2.92 (4H, m), 2.60 (2H, t), 2.30 (2H, t), 1.32-1.14 (1H,m), 0.62-0.54 (2H, m), 0.36-0.28 (2H, m).

Example 96 1-(6-Dimethylaminopyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

To a suspension of 1-(6-chloropyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (90 mg, 0.20 mmol) in methanol (1 ml),the 2.0 M solution of dimethylamine in methanol (0.300 ml, 0.60 mmol)and tetrahydrofuran (0.5 ml) were added and stirred at room temperaturefor 12 hours. The reaction mixture was concentrated under reducedpressure. The residue was diluted with ethyl acetate (50 ml), washedwith H₂O and brine, dried (MgSO₄) and evaporated under reduced pressure.The residue was recrystallized from ethyl acetate/hexane to give thetitle compound (79 mg, 87%).

Example 97 1-(6-Pyrrolidin-1-ylpyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 96

Example 98 1-(6-Morpholin-4-ylpyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 96

Example 99 1-(6-Propoxypyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 96

¹H-NMR (DMSO-d₆) δ: 8.23 (1H, s), 7.68-7.50 (6H, m), 6.56 (1H, d), 5.06(2H, s), 3.30-3.20 (2H, m), 3.10-2.90 (4H, m), 2.65-2.57 (2H, m),2.38-2.22 (2H, m), 1.56 (2H, dt), 0.90 (3H, t).

Example 100 1-(6-Methoxypyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

To a suspension of 1-(6-chloropyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (224 mg, 0.50 mmol) in methanol (5 ml),1N—NaOMe in methanol (3.0 ml, 3.0 mmol) was added under nitrogenatmosphere. The mixture was refluxed for 3 hours. The reaction mixturewas concentrated under reduced pressure. H2O (5 ml) was added, and theresulting precipitate was collected and dried to give the title compound(212 mg, 96%).

Example 101 1-(6-Phenoxypyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 100

¹H-NMR (DMSO-d₆) δ: 8.51 (1H, s), 8.18 (1H, dd), 7.72-7.43 (6H, m),7.32-7.18 (3H, m), 5.08 (2H, s), 3.18-3.04 (4H, m), 2.64 (2H, t), 2.37(2H, t).

Example 102 1-(6-Benzyloxypyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 100

Example 103 1-(6-Propoxypyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 100

Example 104 1-(6-Phenylpyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

To a solution of 1-(6-chloropyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (90 mg, 0.20 mmol) and phenylboronicacid (29 mg, 0.24 mmol) in ethylene glycol dimethyl ether (0.400 ml) andethanol (0.200 ml), tetrakis(triphenylphosphine)palladium (7 mg, 0.006mmol) and 2N aqueous sodium carbonate solution (0.200 ml) were addedunder nitrogen atmosphere and refluxed for 5 hours. H₂O (5 ml) was addedto the reaction mixture and extracted with ethyl acetate (20 ml×2),washed with brine, dried (MgSO₄) and evaporated under reduced pressure.The residue was purified by column chromatography on silica (ethylacetate/hexane, 15/85-40/60) and recrystallized from ethylacetate/hexane to give the title compound (175 mg, 77%).

Example 1055-[4-(3-Trifluoromethylbenzyloxyimino)piperidine-1-sulfonyl]-1H-pyridin-2-one

To a solution of 1-(6-methoxypyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (130 mg, 0.29 mmol) in acetonitrile (4ml), chlorotrimethylsilane (160 mg, 1.47 mmol) in acetonitrile (2 ml)and KI (244 mg, 1.47 mmol) were added and stirred at 80° C. for 1 hour.The reaction mixture was concentrated under reduced pressure. Theresidue was diluted with ethyl acetate (50 ml), washed with H₂O, 10%aqueous Na₂S₂O₃ solution and brine, dried (MgSO₄) and evaporated underreduced pressure. The residue was recrystallized from methanol/H₂O togive the title compound (113 mg, 90%).

Example 106 1-(4-Aminophenylmethanesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

a) A solution of piperidin-4-one O-(3-trifluoromethylbenzyl)oxime (408mg, 1.50 mmol) and triethylamine (0.460 ml, 3.30 mmol) indichloromethane (4 ml), (4-nitrophenyl)methanesulfonyl chloride (390 mg,1.65 mmol) in dichloromethane (2 ml) was slowly added at 0° C. andstirred at room temperature for 1 hour. Saturated aqueous NaHCO₃solution (10 ml) was added, extracted with chloroform (30 ml×2), dried(MgSO₄) and evaporated under reduced pressure to give yellow solid. Thiscrude material was taken up in toluene (13 ml). To the mixture, ironpowder (420 mg, 7.50 mmol), NH₄Cl (802 mg, 15.0 mmol) and H₂O (1.5 ml)was added. The reaction mixture was heated at 105° C. and stirred for 2hours. The reaction mixture was diluted with 30 ml of ethyl acetate,then filtrate through a pad of Celite. The filtrate was concentratedunder reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane, 30/70-60/40) to afford1-(4-aminobenzenesulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (471 mg, 95%, pale yellow oil). To asolution of the free base in ethyl acetate, 4N—HCl in ethyl acetate wasadded. The resulting precipitate was collected and dried in vacuo togive the title compound (417 mg, 63%).

Example 107 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-pyridin-2-ylmethyloxime

a) 4-(Trifluoromethoxy)benzenesulfonyl chloride (4.95 g, 18.6 mmol) wasadded to a solution of 4-piperidone monohydrate hydrochloride (2.92 g,18.6 mmol) and N,N-diisopropylethylamine (9.60 ml, 55.8 mmol) inN,N-dimethylformamide (60 ml) at 0° C. and stirred at room temperaturefor 30 minutes and at 80° C. for 30 minutes. After cooling to roomtemperature, the reaction mixture was diluted with ethyl acetate (150ml), washed with H₂O (50 ml) and brine, dried (MgSO₄) and evaporatedunder reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane 30/70-50/50) to give1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-one as a white solid(3.38 g, 53%, colorless solid).

b) A solution of 1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-one(102 mg, 0.300 mmol), O-pyridin-2-ylmethylhydroxylamine dihydrochloride(59 mg, 0.30 mmol) and sodium acetate (49 mg, 0.60 mmol) in ethanol (3ml) was stirred at room temperature for 30 minutes. The reaction mixturewas concentrated under reduced pressure and the residue was diluted withethyl acetate (30 ml), washed with saturated aqueous NaHCO₃ solution andbrine, dried (MgSO₄) and evaporated under reduced pressure. The residuewas purified by column chromatography on silica (ethyl acetate/hexane30/70-80/20) to give the title compound (117 mg, 91%).

Example 1082-Fluoro-5-[1-(4-trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]benzonitrile

was prepared as described in EXAMPLE 107. Starting material was5-(aminooxymethyl)-2-fluorobenzonitrile (see example A3).

¹H-NMR (DMSO-d₆) δ: 7.90 (2H, d), 7.84 (1H, dd), 7.71-7.70 (1H, m), 7.62(2H, d), 7.48 (1H, t), 5.00 (2H, s), 3.13-3.10 (4H, m), 2.63 (2H, t),2.34 (2H, t).

Example 109 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(4-chlorobenzyl)oxime

was prepared as described in EXAMPLE 107

Example 110 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(6-methoxypyridin-2-ylmethyl)oxime

was prepared as described in EXAMPLE 107. Starting material wasO-((6-methoxypyridin-2-yl)methyl)hydroxylamine (see example A4).

¹H-NMR (DMSO-d₆) δ: 7.91 (2H, d), 7.66-7.62 (3H, m), 6.87 (1H, d), 6.68(1H, d), 4.96 (2H, s), 3.79 (3H, s), 3.14-3.13 (4H, m), 2.68 (2H, t),2.35 (2H, t).

Example 111 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(2-methoxypyridin-3-ylmethyl)oxime

was prepared as described in EXAMPLE 107. Starting material wasO-((2-methoxypyridin-3-yl)methyl)hydroxylamine (see example A5).

¹H-NMR (DMSO-d₆) δ: 8.08 (1H, dd), 7.91 (2H, d), 7.63 (3H, d), 7.58 (3H,dd), 6.94 (1H, dd), 4.94 (2H, s), 3.85 (3H, s), 3.13-3.10 (4H, m), 2.63(2H, t), 2.34 (2H, t).

Example 1123-[1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one

was prepared as described in EXAMPLE 145

Example 1136-[1-(4-Trifluoromethoxy-benzenesulfonyl)-piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one

was prepared as described in EXAMPLE 145

Example 114 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(tetrahydropyran-2-ylmethyl)oxime

was prepared as described in EXAMPLE 107

Example 115 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-cyclohexylmethyloxime

was prepared as described in EXAMPLE 107

Example 116 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-cyclopentylmethyloxime

was prepared as described in EXAMPLE 107

Example 117 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-pyrazin-2-ylmethyloxime

was prepared as described in EXAMPLE 107

Example 118 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(4-chloropyridin-2-ylmethyl)oxime

was prepared as described in EXAMPLE 107

¹H-NMR (DMSO-d₆) δ: 8.48 (1H, d), 7.91 (2H, d), 7.64 (2H, d), 7.43 (1H,dd), 7.33 (1H, d), 5.06 (2H, s), 3.12-3.11 (4H, m), 2.70 (2H, t), 2.35(2H, t).

Example 119 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-[bis(4-fluorophenyl)methyl]oxime

was prepared as described in EXAMPLE 107

¹H-NMR (DMSO-d₆) δ: 7.90 (2H, d), 7.63 (2H, d), 7.34-7.32 (4H, m),7.14-7.11 (4H, m), 6.15 (1H, s), 3.13-3.07 (4H, m), 2.73 (2H, t), 2.30(2H, t).

Example 1202-[1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]benzonitrile

was prepared as described in EXAMPLE 107

¹H-NMR (DMSO-d₆) δ: 7.90 (2H, d), 7.82 (1H, d), 7.64 (3H, dd), 7.52 (2H,dd), 5.14 (2H, s), 3.14-3.08 (4H, m), 2.63 (2H, t), 2.33 (2H, t).

Example 1213-[1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]benzonitrile

was prepared as described in EXAMPLE 107

¹H-NMR (DMSO-d₆) δ: 7.90 (2H, d), 7.74 (2H, d), 7.62 (3H, d), 7.54 (1H,t), 5.03 (2H, s), 3.15-3.08 (4H, m), 2.64 (2H, t), 2.34 (2H, t).

Example 1224-[1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]benzonitrile

was prepared as described in EXAMPLE 107

Example 123 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(4-fluorobenzyl)oxime

was prepared as described in EXAMPLE 107

Example 124 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(2-aminobenzyl)oxime

was prepared as described in EXAMPLE 107

Example 125 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(5-fluoropyridin-2-ylmethyl)oxime

was prepared as described in EXAMPLE 107. Starting material wasO-((5-fluoropyridin-2-yl)methyl)hydroxylamine (see example A6).

Example 126 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(3-fluoropyridin-2-ylmethyl)oxime

was prepared as described in EXAMPLE 107. Starting material wasO-((3-fluoropyridin-2-yl)methyl)hydroxylamine (see example A7).

Example 127 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(5-chloropyridin-2-ylmethyl)oxime

was prepared as described in EXAMPLE 107. Starting material wasO-((5-chloropyridin-2-yl)methyl)hydroxylamine (see example A8).

¹H-NMR (DMSO-d₆) δ: 8.55 (1H, d), 7.91-7.87 (3H, m), 7.63 (2H, d), 7.35(1H, d), 5.05 (2H, s), 3.14 (4H, q), 2.67 (2H, t), 2.34 (2H, t).

Example 128 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(3-dimethylaminobenzyl)oxime

was prepared as described in EXAMPLE 107. Starting material was3-(aminooxymethyl)-N,N-dimethylaniline (see example A9).

¹H-NMR (DMSO-d₆) δ: 7.91-7.88 (2H, m), 7.63 (2H, d), 7.12-7.08 (1H, m),6.62-6.55 (3H, m), 4.91 (2H, s), 3.10 (4H, dt), 2.61 (2H, t), 2.34 (2H,t).

Example 129 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-[1-(4-chlorophenyl)ethyl]oxime

was prepared as described in EXAMPLE 107

Example 130 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-piperidin-3-ylmethyloxime

3-[1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]piperidine-1-carboxylicacid tert-butyl ester (prepared as described in Example 107, 389 mg,0.90 mmol) was dissolve in dichloroethane (5 ml) and cooled to 0° C. Themixture was added trifluoroacetic acid (1 ml) and stirred at 0° C. for30 minutes. The reaction mixture was concentrated under reduced pressureand the residue was diluted with ethyl acetate (60 ml), washed withsaturated aqueous NaHCO₃ solution (20 ml) and brine, dried (MgSO₄) andevaporated under reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/methanol 100/0-80/20) to givethe title compound (216 mg, 55%).

Example 131 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(1-methylpiperidin-3-ylmethyl)oxime

To a solution of 1-(4-trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-piperidin-3-ylmethyloxime (60 mg, 0.14 mmol) in tetrahydrofuran (3ml), formalin (0.014 ml, 0.166 mmol) and sodium triacetoxyborohydride(75 mg, 0.35 mmol) were added and stirred at room temperature for 1hour. The reaction was quenched with saturated aqueous NaHCO₃ solution(5 ml), extracted with chloroform (30 ml×2), dried (MgSO4) andevaporated under reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane 50/50-80/20) to give thetitle compound (59 mg, 95%).

Example 132 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(1-acetylpiperidin-3-ylmethyl)oxime

To a solution of 1-(4-trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-piperidin-3-ylmethyloxime (60 mg, 0.14 mmol) and triethylamine (0.023ml, 0.17 mmol) in dichloroethane (2 ml), acetyl chloride (13 mg, 0.17mmol) was added at 0° C. and stirred at 0° C. for 30 minutes. Thereaction was quenched with saturated aqueous NaHCO₃ solution (5 ml),extracted with chloroform (20 ml×2), dried (MgSO4) and evaporated underreduced pressure. The residue was purified by column chromatography onsilica (ethyl acetate/hexane 40/60-60/40) to give the title compound (61mg, 93%).

Example 133 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(3-aminobenzyl)oxime

was prepared as described in EXAMPLE 107

Example 134 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(4-nitrobenzyl)oxime

was prepared as described in EXAMPLE 107.

¹H-NMR (DMSO-d₆) δ: 8.18 (2H, d), 7.91 (2H, d), 7.63 (2H, d), 7.55 (2H,d), 5.13 (2H, s), 3.14 (4H, q), 2.66 (2H, t), 2.34 (2H, t).

Example 135 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(4-aminobenzyl)oxime

A suspension of 1-(4-trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(4-nitrobenzyl)oxime (200 mg, 0.42 mmol), iron powder (118 mg, 2.11mmol) and NH4Cl (225 mg, 4.2 mmol) in toluene (4 ml) and H₂O (0.3 ml)was stirred at 90° C. overnight. The reaction mixture was filtratedthrough a pad of Celite and the residue was washed with ethylacetate/methanol (4:1). The filtrate was concentrated under reducedpressure and the residue was diluted with chloroform, washed with H₂O,dried (MgSO₄) and evaporated under reduced pressure. The residue waspurified by column chromatography on silica (ethyl acetate/hexane10/90-30/70) to give the title compound (176 mg, 95%).

Example 136 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-piperidin-4-ylmethyloxime

4-[1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]piperidine-1-carboxylicacid tert-butyl ester (prepared as described in Example 107, 273 mg,0.51 mmol) was dissolve in dichloroethane (4 ml) and cooled to 0° C. Themixture was added trifluoroacetic acid (0.38 ml, 5.1 mmol) and stirredat room temperature for 1 hour. The reaction mixture was concentratedunder reduced pressure and the residue was diluted with chloroform,washed with saturated aqueous NaHCO₃ solution (20 ml) and H₂O, dried(MgSO₄) and evaporated under reduced pressure. The residue was purifiedby column chromatography on silica (ethyl acetate/methanol 97/3-70/30)to give the title compound (196 mg, 90%).

Example 137 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(4-aminobenzyl)oxime

was prepared as described in Example 131.

Example 138 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(1-acetylpiperidin-4-ylmethyl)oxime

was prepared as described in Example 132.

Example 139 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(tetrahydropyran-4-ylmethyl)oxime

was prepared as described in Example 107.

Example 1401-Methyl-6-[1-(4-trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one

A suspension of6-[1-(4-trifluoromethoxy-benzenesulfonyl)-piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one(prepared as described in EXAMPLE 113, 60 mg, 0.13 mmol), K₂CO₃ (47 mg,0.34 mmol) and iodomethane (0.50 ml) in acetone was refluxed for 16hours. The reaction mixture was concentrated under reduced pressure andthe residue was diluted with chloroform (60 ml), washed with H₂O (10ml), dried (MgSO₄) and evaporated under reduced pressure. The residuewas purified by column chromatography on silica (ethyl acetate/methanol100/0-90/10) to give the title compound (79 mg, 100%).

Example 1411-Methyl-3-[1-(4-trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one

was prepared as described in Example 140.

Example 142 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(3-methyl-3H-imidazol-4-ylmethyl)oxime

was prepared as described in Example 107.

Example 143 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(5-chlorothiophen-2-ylmethyl)oxime

was prepared as described in Example 107.

Example 144 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(6-methoxypyridin-3-ylmethyl)oxime

was prepared as described in Example 107. Starting material wasO-((6-methoxypyridin-3-yl)methyl)hydroxylamine (see example A10).

¹H-NMR (DMSO-d₆) δ: 8.11 (1H, s), 7.90 (2H, d), 7.65-7.61 (3H, m), 6.77(1H, d), 4.92 (2H, s), 3.83 (3H, s), 3.14-3.07 (4H, m), 2.57 (2H, t),2.34 (2H, t).

Example 1455-[1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one

To a solution of 1-(4-trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(6-methoxypyridin-3-ylmethyl)oxime (492 mg, 1.07 mmol) in acetonitrile(8 ml), chlorotrimethylsilane (350 mg, 3.21 mmol) in acetonitrile (2 ml)and KI (533 mg, 3.21 mmol) were added and refluxed for 2 hour. Thereaction mixture was diluted with chloroform (50 ml), washed with 10%aqueous Na₂S₂O₃ solution, dried (MgSO₄) and evaporated under reducedpressure. The residue was purified by column chromatography on silica(chloroform/methanol 100/0-90/10) to give the title compound (421 mg,89%).

Example 1461-Methyl-5-[1-4-trifluoromethoxy-benzenesulfonyl)-piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one

was prepared as described in Example 140.

Example 147 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(2-chloro-6-methoxypyridin-4-ylmethyl)oxime

was prepared as described in Example 107. Starting material wasO-((2-chloro-6-methoxypyridin-4-yl)methyl)hydroxylamine (see exampleA11).

¹H-NMR (DMSO-d₆) δ: 7.91 (2H, d), 7.63 (2H, d), 6.94 (1H, s), 6.68 (1H,s), 4.99 (2H, s), 3.82 (3H, s), 3.14-3.12 (4H, m), 2.67 (2H, t), 2.34(2H, t).

Example 148 1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-oneO-(2-methoxypyridin-4-ylmethyl)oxime

was prepared as described in Example 107. Starting material wasO-((2-methoxypyridin-4-yl)methyl)hydroxylamine (see example A12).

Example 1496-Chloro-4-[1-(4-trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one

was prepared as described in Example 145.

Example 1504-[1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one

was prepared as described in Example 145.

Example 1511-Methyl-4-[1-(4-trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one

was prepared as described in Example 140.

Example 1526-Chloro-1-methyl-4-[1-(4-trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one

was prepared as described in Example 140.

¹H-NMR (DMSO-d₆) δ: 7.91 (2H, d), 7.63 (2H, d), 6.35 (1H, s), 6.25 (1H,s), 4.82 (2H, s), 3.50 (3H, s), 3.14-3.12 (4H, m), 2.67 (2H, t), 2.35(2H, t).

Example 1532-Fluoro-5-{1-[2-(4-fluorophenyl)acetyl]piperidin-4-ylideneaminooxymethyl}benzonitrile

a) The mixture of 5-(Aminooxymethyl)-2-fluorobenzonitrile hydrochloride(1.74 g, 8.57 mmol), 4-piperidone monohydrate hydrochloride (1.35 g,8.57 mmol) and sodium acetate (1.41 g, 17.2 mmol) in ethanol (60 ml) wasstirred at room temperature for 6 hours. The solvent was evaporatedunder reduced pressure. The residue was diluted with chloroform (100ml), washed with saturated aqueous NaHCO₃ solution (50 ml), dried(MgSO₄) and evaporated under reduced pressure to give2-fluoro-5-((piperidin-4-ylideneaminooxy)methyl)benzonitrile (2.19 g,100%, pale yellow oil).

b) To a solution of2-fluoro-5-((piperidin-4-ylideneaminooxy)methyl)benzonitrile (99 mg,0.40 mmol), 4-fluorophenylacetic acid (68 mg, 0.44 mmol) and1-hydroxybenzotriazole (54 mg, 0.40 mmol) in dichloromethane (4 ml),N-ethyldimethylaminopropylcarbodiimide hydrochloride (92 mg, 0.48 mmol)was added and stirred at room temperature for 2 hours. The reaction wasquenched with saturated aqueous NaHCO₃ solution (10 ml) and extractedwith chloroform (20 ml×2). The organic layer was dried (MgSO₄) andevaporated under reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane, 50/50-100/0) to give thetitle compound (131 mg, 85%).

Example 1542-Fluoro-5-{1-[3-(4-fluorophenyl)propionyl]piperidin-4-ylideneaminooxymethyl}benzonitrile

was prepared as described in Example 153.

Example 1552-Fluoro-5-{1-[(E)-3-(4-fluorophenyl)acryloyl]piperidin-4-ylideneaminooxymethyl}benzonitrile

was prepared as described in Example 153.

Example 1562-Fluoro-5-{1-[2-(4-fluorophenoxy)acetyl]piperidin-4-ylideneaminooxymethyl}benzonitrile

was prepared as described in Example 153.

Example 157 4-(3-Cyano-4-fluorobenzyloxyimino)piperidine-1-carboxylicacid 4-fluorobenzylamide

To a solution of2-fluoro-5-((piperidin-4-ylideneaminooxy)methyl)benzonitrile (99 mg,0.40 mmol) in acetonitrile (4 ml), 4-fluorophenyl isocyanate (67 mg,0.44 mmol) was added and stirred at room temperature for 1 hour. Thereaction was quenched with methanol (10 ml) and the solvent wasevaporated under reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/hexane, 45/55-75/25) to give thetitle compound (90 mg, 57%).

Example 158 4-(3-Cyano-4-fluorobenzyloxyimino)piperidine-1-carboxylicacid 4-fluorophenyl ester

To a solution of2-fluoro-5-((piperidin-4-ylideneaminooxy)methyl)benzonitrile (99 mg,0.40 mmol) and triethylamine (0.061 ml, 0.44 mmol) in dichloromethane (4ml), 4-fluorophenyl chloroformate (78 mg, 0.44 mmol) was added at 0° C.and stirred at 0° C. for 1 hour. The reaction was quenched withsaturated aqueous NaHCO₃ solution (10 ml) and extracted with chloroform(20 ml×2). The organic layer was dried (MgSO₄) and evaporated underreduced pressure. The residue was purified by column chromatography onsilica (ethyl acetate/hexane, 15/85-60/40) to give the title compound(150 mg, 97%).

Example 1595-[1-(2-Aminobenzoyl)piperidin-4-ylideneaminooxymethyl]-2-fluorobenzonitrile

was prepared as described in Example 153.

Example 160 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(1-methyl-1H-benzo[d]imidazol-2-yl)methyl oxime

was prepared as described in Example 107.

¹H-NMR (DMSO-d₆) δ: 7.89 (2H, d), 7.60-7.54 (4H, m), 7.26-7.19 (2H, m),5.25 (2H, s), 3.78 (3H, s), 3.15-3.08 (4H, m), 2.61 (2H, t), 2.33 (2H,t).

Example 161 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(1-methyl-1H-imidazol-2-yl)methyl oxime

was prepared as described in Example 107.

Example 162 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(1H-benzo[d]imidazol-2-yl)methyl oxime

To a solution of tert-Butyl2-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)-1H-benzo[d]imidazole-1-carboxylate(prepared as described in Example 107, 275 mg, 0.484 mmol) indichloromethane (8 ml), trifluoroacetic acid (4 ml) was added at 0° C.and stirred at room temperature for 2 hours. The solvent was removedunder reduced pressure. Saturated aqueous NaHCO₃ solution (10 ml) wasadded and extracted with chloroform. The organic layer was washed withH₂O, dried (Na₂SO₄) and evaporated under reduced pressure. The residualsolid was triturated with ethyl acetate/methanol (90/10) to give thetitle compound (160 mg, 70%).

¹H-NMR (DMSO-d₆) δ: 12.32 (1H, s), 7.90 (2H, t), 7.62 (2H, d), 7.48 (2H,br), 7.16 (2H, d), 5.15 (2H, s), 3.12 (4H, q), 2.67 (2H, t), 2.35 (2H,t).

Example 1635-((1-(3,3-Bis(4-fluorophenyl)acryloyl)piperidin-4-ylideneaminooxy)methyl)-2-fluorobenzonitrile

was prepared as described in Example 153.

¹H-NMR (DMSO-d₆) δ: 7.86 (1H, t), 7.73 (1H, d), 7.52 (1H, t), 7.33 (2H,t), 7.22 (6H, m), 6.56 (1H, s), 5.02 (2H, s), 3.45 (4H, t), 2.41 (1H,t), 2.19 (2H, dt), 1.98 (1H, t).

Example 1645-((1-(3,3-Bis(4-fluorophenyl)propanoyl)piperidin-4-ylideneaminooxy)methyl)-2-fluorobenzonitrile

was prepared as described in Example 153.

¹H-NMR (DMSO-d₆) δ: 7.87 (1H, d), 7.75 (1H, t), 7.52 (1H, t), 7.35 (4H,dd), 7.08 (4H, t), 5.03 (2H, s), 4.53 (1H, t), 3.63-3.57 (2H, m), 3.45(2H, q), 3.15 (2H, t), 2.47-2.39 (2H, m), 2.19 (2H, dt).

Example 1655-((1-(6-(Cyclopropylamino)pyridin-3-ylsulfonyl)piperidin-4-ylideneaminooxy)methyl)-2-fluorobenzonitrile

was prepared as described in EXAMPLE 96

Example 1662-Fluoro-5-((1-(2-(4-fluorophenylamino)acetyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in Example 153.

Example 1672-(4-(3-Cyano-4-fluorobenzyloxyimino)piperidin-1-yl)-N-(4-fluorophenyl)acetamide

The mixture of2-fluoro-5-((piperidin-4-ylideneaminooxy)methyl)benzonitrile (172 mg,0.696 mmol), 2-bromo-N-(4-fluorophenyl)acetamide (194 mg, 0.835 mmol)and K₂CO₃ (115 mg, 0.835 mmol) in acetonitrile (7 ml) was stirred atroom temperature for 1 hour. The solvent was evaporated under reducedpressure and the residue was diluted with ethyl acetate (60 ml), washedwith H₂O (10 ml) and brine, dried (MgSO₄) and evaporated under reducedpressure. The residue was purified by column chromatography on silica(ethyl acetate/hexane, 50/50-70/30) to give the title compound (120 mg,68%).

Example 1685-((1-(4-Aminophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)-2-fluorobenzonitrile

was prepared as described in Example 83.

Example 1692-(Cyclopropylamino)-5-((1-(4-fluorophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

The mixture of2-fluoro-5-((1-(4-fluorophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile(200 mg, 0.493 mmol) and cyclopropylamine (2 ml) was refluxed for 4days. The solvent was evaporated under reduced pressure and the residuewas diluted with ethyl acetate (60 ml), washed with H₂O (10 ml) andbrine, dried (MgSO₄) and evaporated under reduced pressure. The residuewas purified by column chromatography on silica (ethyl acetate/hexane,15/85-35/65) to give the title compound (65 mg, 30%).

Example 1702-(Cyclopropylmethylamino)-5-((1-(4-(cyclopropylmethylamino)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

The mixture of2-fluoro-5-((1-(4-fluorophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile(200 mg, 0.493 mmol) and aminomethylcyclopropane (0.65 ml) was refluxedfor 3 days. The solvent was evaporated under reduced pressure and theresidue was diluted with ethyl acetate (60 ml), washed with H₂O (10 ml)and brine, dried (MgSO₄) and evaporated under reduced pressure. Theresidue was purified by column chromatography on silica (ethylacetate/hexane, 30/70-60/40) to give the title compound (201 mg, 80%).

Example 171N-(4-(4-(3-Cyano-4-fluorobenzyloxyimino)piperidin-1-ylsulfonyl)phenyl)acetamide

To a solution of5-((1-(4-Aminophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)-2-fluorobenzonitrile(100 mg, 0.248 mmol) and triethylamine (0.042 ml, 0.30 mmol) intetrahydrofuran (3 ml), acetyl chloride (0.088 ml, 1,2 mmol) was addedat 0° C. and stirred at room temperature for 2 hours. H₂O (10 ml) wasadded, extracted with ethyl acetate (30 ml×2), washed with brine, dried(MgSO₄) and evaporated under reduced pressure. The residue was purifiedby column chromatography on silica (ethyl acetate/hexane, 65/35-100/0)to give the title compound (96 mg, 87%).

Example 172 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(3-methyl-4,5-dihydroisoxazol-5-yl)methyl oxime

was prepared as described in Example 107.

Example 1736-((1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)picolinonitrile

was prepared as described in Example 107.

¹H-NMR (DMSO-d₆) δ: 8.02 (1H, t), 7.93 (3H, t), 7.64 (3H, dd), 5.10 (2H,s), 3.14 (4H, t), 2.69 (2H, t), 2.34 (2H, t).

Example 174 (R)-1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-morpholin-3-ylmethyl oxime

was prepared as described in Example 107: Starting material was(R)-tert-butyl 3-(aminooxymethyl)morpholine-4-carboxylate (see exampleA13).

Example 175 (S)-1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-morpholin-3-ylmethyl oxime

was prepared as described in Example 107. Starting material was(S)-tert-butyl 3-(aminooxymethyl)morpholine-4-carboxylate (see exampleA14).

Example 1762-Fluoro-5-((1-(4-(methylamino)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in Example 107.

a) To a solution of5-((1-(4-Aminophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)-2-fluorobenzonitrile(201 mg, 0.500 mmol) in tetrahydrofuran (6 ml), trifluoroaceticanhydride (0.085 ml, 0.6 mmol) was added at 0° C. and stirred at 0° C.for 30 minutes. The reaction was quenched with saturated aqueous NaHCO₃solution (10 ml), extracted with diethyl ether (30 ml×2), dried (MgSO4)and evaporated under reduced pressure to giveN-(4-(4-(3-cyano-4-fluorobenzyloxyimino)piperidin-1-ylsulfonyl)phenyl)-2,2,2-trifluoroacetamide(248 mg, 100%, colorless solid).

b) To a solution ofN-(4-(4-(3-cyano-4-fluorobenzyloxyimino)piperidin-1-ylsulfonyl)phenyl)-2,2,2-trifluoroacetamide(100 mg, 0.200 mmol) and iodomethane (0.050 ml, 0.80 mmol) in acetone (1ml), potassium hydroxide (45 mg, 0.80 mmol) and H₂O (1 ml) was added at60° C. and refluxed for 1 hour. The reaction mixture was diluted with 40ml of ethyl acetate and washed with H₂O (10 ml) and brine. The organiclayer was dried over MgSO₄ and concentrated. The residue was purified bycolumn chromatography on silica (ethyl acetate/methanol, 40/60-60/40) togive the title compound (65 mg, 78%).

Example 1774-((1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)picolinonitrile

was prepared as described in Example 107.

¹H-NMR (DMSO-d₆) δ: 8.69 (1H, d), 7.92-7.91 (3H, m), 7.64-7.62 (3H, m),5.11 (2H, s), 3.15-3.13 (4H, m), 2.70 (2H, s), 2.34 (2H, s).

Example 1782-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107. Starting material was2-(aminooxymethyl)isonicotinonitrile (see example A15).

¹H-NMR (DMSO-d₆) δ: 8.77 (1H, d), 7.92 (2H, d), 7.77 (1H, d), 7.72 (1H,s), 7.64 (2H, d), 5.12 (2H, s), 3.15-3.13 (4H, m), 2.71 (2H, t), 2.35(2H, t).

Example 179 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(4-methoxypyridin-2-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((4-methoxypyridin-2-yl)methyl)hydroxylamine (see example A16).

Example 1805((1-(2-(Bis(4-fluorophenyl)amino)acetyl)piperidin-4-ylideneaminooxy)methyl)-2-fluorobenzonitrile

was prepared as described in Example 153.

Example 1815-((1-(4,4-Bis(4-fluorophenyl)butanoyl)piperidin-4-ylideneaminooxy)methyl)-2-fluorobenzonitrile

was prepared as described in Example 153.

¹H-NMR (DMSO-d₆) δ: 7.88-7.87 (1H, m), 7.75-7.73 (1H, m), 7.52 (1H, t),7.32 (4H, t), 7.10 (4H, t), 5.04 (2H, s), 4.01 (1H, s), 3.52 (2H, q),3.37 (2H, d), 2.24 (6H, t).

Example 1825-((1-(Bis(4-fluorophenyl)methyl)piperidin-4-ylideneaminooxy)methyl)-2-fluorobenzonitrilehydrochloride

a) The mixture of2-fluoro-5-((piperidin-4-ylideneaminooxy)methyl)benzonitrile (124 mg,0.500 mmol), 4,4′-(chloromethylene)bis(fluorobenzene) (122 mg, 0.500mmol), KI (8 mg, 0.05 mmol) and K₂CO₃ (83 mg, 0.60 mmol) in acetonitrile(5 ml) was refluxed for 14 hours. The reaction was quenched with H₂O,extracted with chloroform (30 ml×2), dried (MgSO₄) and concentrated. Theresidue was purified by column chromatography on silica (ethylacetate/methanol, 10/90-35/65) to give5-((1-(bis(4-fluorophenyl)methyl)piperidin-4-ylideneaminooxy)methyl)-2-fluorobenzonitrile(195 mg, colorless oil). To a solution of this free base in 1,4-dioxane(2 ml), 4N—HCl in 1,4-dioxane (1 ml) was added and stirred at roomtemperature for 30 minutes. The solvent was removed under reducedpressure to give the title compound (225 mg, 92%).

¹H-NMR (DMSO-d₆) δ: 7.97-7.92 (5H, m), 7.78-7.75 (1H, m), 7.53 (1H, t),7.33-7.30 (4H, m), 5.76 (1H, d), 5.07 (2H, s), 3.32-2.82 (8H, m).

Example 183N-(Bis-4-fluorophenyl-methyl)-4-(3-cyano-4-fluorobenzyloxyimino)piperidine-1-carboxamide

To a solution of bis(4-fluorophenyl)methanamine (110 mg, 0.500 mmol) andpyridine (0.036 ml, 0.500 mmol) in dichloromethane (5 ml), chloroformicacid 4-nitrophenyl ester (101 mg, 0.500 mmol) was added at 0° C. andstirred for 30 minutes. Triethylamine (0.070 ml, 0.50 mmol) and asolution of 2-fluoro-5-((piperidin-4-ylideneaminooxy)methyl)benzonitrile(124 mg, 0.500 mmol) in dichloromethane (3 ml) was added to the reactionmixture and stirred at room temperature for 5 hour. The reaction wasquenched with H₂O, extracted with chloroform (30 ml×2), dried (MgSO₄)and concentrated. The residue was purified by column chromatography onsilica (ethyl acetate/methanol, 50/50-70/30) to give the title compound(158 mg, 70%).

Example 184 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-isoquinolin-1-yl oxime

was prepared as described in Example 107. Starting material wasO-(isoquinolin-1-yl)hydroxylamine (see example A17).

Example 185 1-(Bis(4-fluorophenyl)methyl)piperidin-4-one O-benzhydryloxime

was prepared as described in Example 183.

Example 1863-(Cyclopropyl(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in Example 107. Starting material was3-(aminooxy(cyclopropyl)methyl)benzonitrile (see example A18).

¹H-NMR (DMSO-d₆) δ: 7.90 (2H, d), 7.70 (2H, d), 7.64-7.61 (3H, m), 7.51(1H, t), 4.42 (1H, d), 3.19-2.98 (4H, m), 2.73-2.66 (2H, m), 2.29-2.23(2H, m), 1.14-1.10 (1H, m), 0.60-0.37 (4H, m).

Example 187 Methyl6-(4-(3-cyano-4-fluorobenzyloxyimino)piperidin-1-ylsulfonyl)-1H-benzo[d]imidazol-2-ylcarbamate

To a solution of2-fluoro-5-((piperidin-4-ylideneaminooxy)methyl)benzonitrile (247 mg,1.00 mmol) and triethylamine (0.35 ml, 2.5 mmol) in dichloromethane (5ml), methyl 6-(chlorosulfonyl)-1H-benzo[d]imidazol-2-ylcarbamate (326mg, 1.00 mmol) was added at 0° C. and stirred at room temperature for 3hours. The reaction was quenched with H₂O, extracted withdichloromethane, dried (MgSO4) and evaporated under reduced pressure.The residual solid was triturated with diethyl ether/hexane (4/1) togive the title compound (466 mg, 93%).

Example 1885-((1-(2-Amino-1H-benzo[d]imidazol-6-ylsulfonyl)piperidin-4-ylideneaminooxy)methyl)-2-fluorobenzonitrile

To a solution of methyl6-(4-(3-cyano-4-fluorobenzyloxyimino)piperidin-1-ylsulfonyl)-1H-benzo[d]imidazol-2-ylcarbamate(150 mg, 0.300 mmol) in ethylene glycol (1.5 ml) and H₂O (0.4 ml),potassium hydroxide (50 mg, 0.90 mmol) was added and stirred at 95° C.for 90 minutes. The reaction was quenched with H₂O and the precipitatedmaterial was collected, then purified by column chromatography on silica(ethyl acetate/methanol, 90/10-70/30) to give the title compound (50 mg,40%).

Example 189 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(4-methoxyquinolin-2-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((4-methoxyquinolin-2-yl)methyl)hydroxylamine (see example A19).

¹H-NMR (DMSO-d₆) δ: 8.09 (1H, d), 7.91-7.87 (3H, m), 7.72 (1H, dd), 7.64(2H, d), 7.53 (1H, dd), 6.88 (1H, s), 5.17 (2H, s), 3.95 (3H, s),3.14-3.13 (4H, m), 2.76 (2H, t), 2.36 (2H, t).

Example 190 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(4-fluorophenyl)(6-methoxypyridin-3-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((4-fluorophenyl)(6-methoxypyridin-3-yl)methyl)hydroxylamine (seeexample A20).

Example 1913-(2-Hydroxy-1-(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)ethyl)benzonitrile

To a solution of3-(2-(tert-butyldimethylsilyloxy)-1-(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)ethyl)benzonitrile(prepared as described in Example 107 starting from3-(1-(aminooxy)-2-(tert-butyldimethylsilyloxy)ethyl)benzonitrile (seeexample A21), 154 mg, 0.250 mmol) in tetrahydrofuran (5 ml),tetra-n-butylammonium fluoride hydrate (131 mg, 0.500 mmol) was addedand stirred at room temperature for 30 minutes. The solvent wasevaporated under reduced pressure and the residue was diluted with ethylacetate (60 ml), washed with saturated aqueous NaHCO₃ solution (10 ml)and brine, dried (MgSO₄) and evaporated under reduced pressure. Theresidue was purified by column chromatography on silica (ethylacetate/hexane, 55/45-75/25) to give the title compound (104 mg, 86%).

¹H-NMR (DMSO-d₆) δ: 7.91 (2H, d), 7.69-7.61 (5H, m), 7.51 (1H, t),5.06-5.03 (1H, m), 4.92-4.90 (1H, m), 3.64-3.60 (2H, m), 3.11-3.10 (4H,m), 2.76-2.70 (2H, m), 2.31-2.29 (2H, m).

Example 192 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(5-chlorobenzo[d]oxazol-2-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((5-chlorobenzo[d]oxazol-2-yl)methyl)hydroxylamine (see example A22).

Example 1932-((1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)quinolin-4(1H)-one

was prepared as described in Example 145.

Example 1942-((1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)pyridin-4(1H)-one

was prepared as described in Example 145.

Example 195 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-benzhydryl oxime

was prepared as described in Example 107.

Example 1963-((1-(4-Fluorophenylsulfonyl)piperidin-4-ylideneaminooxy)methylbenzonitrile

was prepared as described in EXAMPLE 50

Example 1973-((1-(4-(Difluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 1983-((1-(4-Methoxyphenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 1993-((1-(4-Cyanophenylsulfonyl)piperidin-4-ylideneaminooxymethyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 200 N-Benzhydryl-4-(benzhydryloxyimino)piperidine-1-carboxamide

was prepared as described in EXAMPLE 183

Example 201N-Benzhydryl-4-(3-cyanobenzyloxyimino)piperidine-1-carboxamide

was prepared as described in EXAMPLE 183

Example 2024-(3-Cyanobenzyloxyimino)-N-(9H-fluoren-9-yl)piperidine-1-carboxamide

was prepared as described in EXAMPLE 183

Example 203 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(1-(2-hydroxyethyl)-1H-benzo[d]imidazol-2-yl)methyl oxime

a) To a solution of1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(1H-benzo[d]imidazol-2-yl)methyl oxime (134 mg, 0.290 mmol) inN,N-dimethylformamide (2 ml), NaH (60%, 13 mg, 0.31 mmol) was added at0° C. and stirred at room temperature for 10 minutes.tert-Butyl-(2-bromoethoxy)dimethylsilane (0.067 ml, 0.31 mmol) was addedto the reaction mixture and stirred at room temperature for 3 hours. Thereaction was quenched with H₂O and extracted with ethyl acetate, dried(MgSO₄) and evaporated under reduced pressure. The residue was purifiedby column chromatography on silica (ethyl acetate/hexane, 30/70-50/50)to give 1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(1-(2-(tert-butyldimethylsilyloxy)ethyl)-1H-benzo[d]imidazol-2-yl)methyloxime (137 mg, 75%, pale yellow oil).

b) To a solution of1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(1-(2-(tert-butyldimethylsilyloxy)ethyl)-1H-benzo[d]imidazol-2-yl)methyloxime (137 mg, 0.220 mmol) in tetrahydrofuran (3 ml),tetra-n-butylammonium fluoride hydrate (1 M solution in tetrahydrofuran,0.26 ml, 0.26 mmol) was added at 0° C. and stirred at room temperaturefor 15 minutes. The reaction was quenched with H₂O and extracted withethyl acetate, dried (MgSO₄) and evaporated under reduced pressure. Theresidue was purified by column chromatography on silica(chloroform/methanol, 95/5-90/10) to give the title compound (94 mg,80%).

Example 204 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(1H-indol-2-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((1H-indol-2-yl)methyl)hydroxylamine (see example A23).

Example 2053-((1-(3,4-Dimethoxyphenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2063-((1-(2,5-Dimethoxyphenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2075-(4-(3-Cyanobenzyloxyimino)piperidin-1-ylsulfonyl)-2-fluorobenzonitrile

was prepared as described in EXAMPLE 50

Example 2083-((1-(3,5-Difluorophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2093-((1-(2,4-Difluorophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2103-((1-(3,4-Difluorophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2113-((1-(2,5-Difluorophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 212 Methyl3-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzoate

was prepared as described in Example 107.

Example 2133-((1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzoicacid

To a solution of methyl3-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzoate(1.08 g, 2.22 mmol) in methanol (15 ml), aqueous sodium hydroxidesolution (4 M, 1.10 ml, 4.40 mmol) was added and refluxed for 1 hour.HCl (1 M solution, 5 ml) and H₂O (10 ml) was added dropwise to thereaction mixture, and the resulting precipitate was collected, washedwith H₂O (10 ml×3) and diethyl ether (5 ml×3) to give the title compound(875 mg, 83%)

Example 2145-((4-Fluorophenyl)(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)pyridin-2(1H)-one

was prepared as described in Example 145.

¹H-NMR (DMSO-d₆) δ: 11.50 (1H, br s), 7.90 (2H, d), 7.63 (2H, d),7.32-7.29 (3H, m), 7.23 (1H, s), 7.14 (2H, t), 6.26 (1H, d), 5.93 (1H,s), 3.12-3.07 (4H, m), 2.72-2.67 (2H, m), 2.31 (2H, t).

Example 215 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(4-fluorophenyl)(1-methyl-1H-imidazol-5-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((4-Fluorophenyl)(1-methyl-1H-imidazol-5-yl)methyl)hydroxylamine (seeexample A24).

Example 216 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(4-fluorophenyl)(piperidin-4-yl)methyl oxime

To a solution of tert-Butyl4-((4-fluorophenyl)(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)piperidine-1-carboxylate(prepared as described in Example 107 starting from tert-butyl4-(aminooxy(4-fluorophenyl)methyl)piperidine-1-carboxylate (see exampleA25), 200 mg, 0.317 mmol) in dichloroethane (2 ml), trifluoroacetic acid(1 ml) was added at 0° C. and stirred at 0° C. for 2 hours. The reactionmixture was concentrated under reduced pressure and the residue wasdiluted with ethyl acetate, washed with saturated aqueous NaHCO₃solution and brine, dried (MgSO₄) and evaporated under reduced pressureto give the title compound (172 mg, 100%).

¹H-NMR (DMSO-d₆) δ: 7.90 (2H, d), 7.63 (2H, d), 7.18-7.07 (4H, m), 4.72(1H, d), 3.06-2.90 (6H, m), 2.67 (2H, t), 2.39-2.19 (4H, m), 1.74-1.68(2H, m), 1.12-1.04 (3H, m).

Example 217 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(1H-indol-3-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((1H-indol-3-yl)methyl)hydroxylamine (see example A26).

Example 2183-((1-(4-(2-Methoxyethylamino)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 86

Example 2193-((1-(4-(2-Methoxyethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 91

Example 2203-((1-(4-(2-Hydroxyethylamino)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 86

Example 2213-((1-(4-(2-Hydroxyethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

To a solution of3-((1-(4-(2-(tetrahydro-2H-pyran-2-yloxy)ethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile(prepared as described in EXAMPLE 91, 466 mg, 0.516 mmol) intetrahydrofuran (1.5 ml) and methanol (5 mL) was added a catalyticamount of camphorsulfonic acid (50 mg) at 0° C. After being stirred for2 hours at room temperature, the reaction mixture was diluted with ethylacetate and poured into saturated aqueous NaHCO₃ at 0° C. The aqueouslayer was extracted with ethyl acetate and the combined extracts werewashed with H₂O and brine, dried over Na₂SO4, filtered and evaporated invacuo. The residue was purified by column chromatography on silica(ethyl acetate/hexane, 50/50-80/20) and recrystallized fromisopropylether/chloroform to give the title compound (184 mg, 83%).

Example 2223-((1-(4-(Cyclopropylmethylamino)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 86

Example 2233-((1-(4-(2-Hydroxy-2-methylpropylamino)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 86

Example 224N-(3,5-Bis(trifluoromethylphenyl)-4-(3-(trifluoromethyl)benzyloxyimino)piperidine-1-carboxamide

was prepared as described in EXAMPLE 183

Example 2254-(Bis(4-fluorophenyl)methoxyimino)-N-(3,5-bis(trifluoromethyl)phenyl)piperidine-1-carboxamide

was prepared as described in EXAMPLE 183

Example 226N-(2,4-Difluorophenyl)-3-oxo-3-(4-(3-(trifluoromethyl)benzyloxyimino)piperidin-1-yl)propanamide

was prepared as described in Example 153.

Example 2273-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-yl)-N-(2,4-difluorophenyl)-3-oxopropanamide

was prepared as described in Example 153.

Example 228 1-(2,4-Dichlorophenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 2292-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-ylsulfonyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 230 1-(o-Tolylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 231 1-(4-Butylphenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 232 1-(4-(Difluoromethoxy)phenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 233 1-(3-(Difluoromethoxy)phenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 234 1-(1-Methyl-1H-indol-4-ylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 235 1-(4-(1H-Pyrazol-1-yl)phenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 236 1-(Benzo[d][1,3]dioxol-5-ylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 2371-(4-Methyl-3,4-dihydro-2H-benzo[b][1,4]oxazin-7-ylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 238 1-(2-Methoxyphenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 2393-((1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzamide

To a solution of3-((1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzoicacid (150 mg, 0.318 mmol), 1-hydroxybenzotriazole (46.4 mg, 0.343 mmol),NH4Cl (34.9 mg, 0.652 mmol) and N,N-diisopropylethylamine (0.220 ml,1.26 mmol) in N,N-dimethylformamide,N-ethyldimethylaminopropylcarbodiimide hydrochloride (74.5 mg, 0.389mmol) was added and stirred at room temperature for 88 hours. H₂O (3 ml)was added dropwise to the reaction mixture at room temperature andstirred at 0° C. for 30 minutes. The resulting precipitate wascollected, washed with H₂O (5 ml×3) and dried under reduced pressure at50° C. to give the title compound (135 mg, 90%).

Example 240N-Methyl-3-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzamide

was prepared as described in EXAMPLE 239

Example 241N,N-Dimethyl-3-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzamide

was prepared as described in EXAMPLE 239

Example 242 1-(3,5-Dimethylisoxazol-4-ylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 243 1-(3,4-Difluorophenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 244 1-(3,5-Difluorophenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 245 1-(2,4-Difluorophenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 246 1-(4-Fluorophenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 247 1-(4-Butylphenylsulfonyl)piperidin-4-oneO-3-chloro-5-fluorobenzyl oxime

was prepared as described in EXAMPLE 65

Example 248 1-(4-Butylphenylsulfonyl)piperidin-4-one O-cyclopropylmethyloxime

was prepared as described in EXAMPLE 65

Example 249 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-cyclopropylmethyl oxime

was prepared as described in EXAMPLE 65

Example 250 1-(3-(Trifluoromethyl)-phenylsulfonyl)piperidin-4-oneO-cyclopropylmethyl oxime

was prepared as described in EXAMPLE 65

Example 251 1-(Quinolin-8-ylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 252 1-(Thiophen-2-ylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 2534-(Bis(4-fluorophenyl)methoxyimino)-N,N-dimethylpiperidine-1-sulfonamide

was prepared as described in EXAMPLE 50

Example 254 1-(1-Methyl-1H-imidazol-4-ylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 255 1-(Cyclopropylsulfonyl)-piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 2564-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-ylsulfonyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2575-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-ylsulfonyl)-2-fluorobenzonitrile

was prepared as described in EXAMPLE 50

Example 258 1-(2,5-Dimethoxyphenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 259 1-(2,5-Difluorophenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 260 1-(4-Methoxyphenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 2611-(2,3-Dihydrobenzo[b][1,4]dioxin-5-ylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 262 1-(1,2-Dimethyl-1H-imidazol-4-ylsulfonyl)-piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 263 (S)-1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-indolin-2-ylmethyl oxime

To a solution of (S)-tert-butyl2-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)indoline-1-carboxylate(prepared as described in Example 107 starting from (S)-tert-butyl2-(aminooxymethyl)indoline-1-carboxylate (see example A27), 160 mg,0.280 mmol) in dichloroethane (2 ml), trifluoroacetic acid (0.42 ml,5.62 mmol) was added and stirred at room temperature for 45 minutes. Thereaction mixture was quenched with ammonia solution at 0° C., extractedwith chloroform, dried (MgSO₄) and evaporated under reduced pressure.The residue was purified by column chromatography on silica (ethylacetate/hexane, 20/80-60/40) to give the title compound (125 mg, 95%).

¹H-NMR (DMSO-d₆) δ: 7.91 (2H, d), 7.65 (2H, d), 6.92 (1H, d), 6.77 (1H,d), 6.40 (2H, dd), 5.55 (1H, s), 3.92 (3H, s), 3.09-3.00 (5H, m), 2.55(3H, t), 2.32 (2H, t).

Example 264 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(1H-benzo[d]imidazol-5-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((1H-benzo[d]imidazol-6-yl)methyl)hydroxylamine (see example A28).

Example 265 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-benzo[d][1,3]dioxol-2-ylmethyl oxime

was prepared as described in Example 107. Starting material wasO-(benzo[d][1,3]dioxol-2-ylmethyl)hydroxylamine (see example A29).

¹H-NMR (DMSO-d₆) δ: 7.88 (2H, d), 7.69 (2H, d), 6.74 (2H, dd), 6.49 (2H,dd), 6.40 (1H, t), 4.24 (2H, d), 3.01 (2H, t), 2.71 (2H, t), 2.30 (4H,td).

Example 266 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(6-fluoro-1H-benzo[d]imidazol-2-yl)methyl oxime

was prepared as described in Example 162. Starting material wastert-Butyl2-(aminooxymethyl)-5-fluoro-1H-benzo[d]imidazole-1-carboxylate (seeexample A30).

Example 2673-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-ylsulfonyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 268 1-(3,4-Dimethoxyphenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 2693-(Pyridin-4-yl(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in Example 107. Starting material was3-(aminooxy(pyridin-4-yl)methyl)benzonitrile (see example A31).

¹H-NMR (DMSO-d₆) δ: 8.62-8.61 (1H, m), 8.47 (1H, d), 7.89 (3H, t), 7.72(3H, t), 7.63 (2H, d), 7.55 (1H, t), 7.34 (1H, dd), 6.29 (1H, s),3.15-3.09 (4H, m), 2.79 (2H, t), 2.32 (2H, t).

Example 2703-(Pyridin-3-yl(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in Example 107. Starting material was3-(aminooxy(pyridin-3-yl)methyl)benzonitrile (see example A32).

¹H-NMR (DMSO-d₆) δ: 8.51 (2H, m), 7.90 (3H, t), 7.64 (5H, m), 7.38 (2H,d), 6.24 (1H, s), 3.13 (4H, m), 2.81 (2H, t), 2.32 (2H, t).

Example 2713-(Pyridin-2-yl(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in Example 107. Starting material was3-(aminooxy(pyridin-2-yl)methyl)benzonitrile (see example A33).

¹H-NMR (DMSO-d₆) δ: 8.47 (1H, d), 7.91 (2H, d), 7.82-7.68 (4H, m), 7.63(2H, d), 7.53-7.49 (2H, m), 7.27 (1H, dd), 6.19 (1H, s), 3.14-3.11 (4H,m), 2.80 (2H, t), 2.32 (2H, t).

Example 2723-((1-(6-Chloropyridin-3-ylsulfonyl)piperidin-4-ylideneaminooxy)(cyclopropyl)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2733-(2-Methoxy-1-(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)ethyl)benzonitrile

A solution of3-(2-hydroxy-1-(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)ethyl)benzonitrile(80 mg, 0.16 mmol) and iodomethane (0.040 ml, 0.65 mmol) intetrahydrofuran (4 ml) was added dropwise to a suspension of NaH (60%,10 mg, 0.24 mmol) in tetrahydrofuran (1 ml) at 0° C. and stirred at roomtemperature for 2 hours. The reaction was quenched with H₂O (10 ml) andextracted with diethyl ether (20 ml×2). The organic layer was washedwith brine, dried (MgSO₄) and evaporated under reduced pressure. Theresidue was purified by column chromatography on silica (ethylacetate/hexane, 30/70-50/50) to give the title compound (77 mg, 96%).

Example 2743-(Cyclopropyl(1-(6-(cyclopropylamino)pyridin-3-ylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 96

Example 2753-((1-(6-(Cyclopentylamino)pyridin-3-ylsulfonyl)piperidin-4-ylideneaminooxy)(cyclopropyl)methyl)benzonitrile

was prepared as described in EXAMPLE 96

Example 276 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-1-phenylethyl oxime

was prepared as described in EXAMPLE 65

Example 277 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-cyclohexylmethyl oxime

was prepared as described in EXAMPLE 65

Example 2785-(4-((3-Cyanophenyl)(cyclopropyl)methoxyimino)piperidin-1-ylsulfonyl)picolinonitrile

To a solution of3-((1-(6-Chloropyridin-3-ylsulfonyl)piperidin-4-ylideneaminooxy)(cyclopropyl)methyl)benzonitrile(167 mg, 0.375 mmol) in N,N-dimethylformamide (2 ml), zinc cyanide (33mg, 0.28 mmol) and tetrakis(triphenylpshosphine)palladium(0) (44 mg,0.039 mmol) were added and stirred at 100° C. for 7 hours. The reactionwas quenched with saturated aqueous K₂CO₃ solution and extracted withdiethyl ether (30 ml×2). The organic layer was washed with brine, dried(MgSO₄) and evaporated under reduced pressure. The residue was purifiedby column chromatography on silica (ethyl acetate/hexane, 30/70-50/50)to give the title compound (97 mg, 60%).

¹H-NMR (DMSO-d₆) δ: 9.08 (1H, d), 8.43 (1H, dd), 8.31 (1H, d), 7.72-7.71(2H, m), 7.63 (1H, d), 7.53 (1H, t), 4.42 (1H, d), 3.26-3.15 (4H, m),2.70 (2H, t), 2.27 (2H, t), 1.18-1.11 (1H, m), 0.59-0.38 (4H, m).

Example 2793-((1-(Benzo[d][1,3]dioxol-5-ylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2803-((1-(4-(Trifluoromethyl)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2813-((1-(4-(2-Fluoroethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2823-(4-(3-Cyanobenzyloxyimino)piperidin-1-ylsulfonyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2833-((1-(Quinolin-8-ylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 2843-(4-(3-(Trifluoromethyl)benzyloxyimino)piperidin-1-ylsulfonyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 285 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 286 Methyl3-(4-(bis(4-fluorophenyl)methoxyimino)piperidin-1-ylsulfonyl)benzoate

was prepared as described in EXAMPLE 50

Example 287 1-(Thiophen-3-ylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 288 1-(Pyridin-2-ylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 289 1-(2-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 290 1-(3-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 291 1-(Pyridin-3-ylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 292 1-(3-Chlorophenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in EXAMPLE 50

Example 2933-((1-(4-(2-Cyanoethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 294 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-2-cyclohexylethyl oxime

was prepared as described in EXAMPLE 65

Example 2951-(4-Fluorobenzyl)-5-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)pyridin-2(1H)-one

To a solution of5-[1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one(133 mg, 0.300 mmol), K₂CO₃ (104 mg, 0.750 mmol) and KI (5 mg, 0.03mmol) in DME (10 ml), 4-fluorobenzyl bromide (0.112 ml, 0.900 mmol) wasadded and refluxed for 60 hours. The reaction was quenched with H₂O (15ml) and extracted with ethyl acetate (30 ml×2). The organic layer waswashed with brine, dried (MgSO₄) and evaporated under reduced pressure.The residue was purified by column chromatography on silica (ethylacetate/hexane, 80/20-100/0) to give the title compound (125 mg, 75%).

¹H-NMR (DMSO-d₆) δ: 7.89 (2H, d), 7.82 (1H, d), 7.62 (2H, d), 7.39-7.35(3H, m), 7.14 (2H, t), 6.38 (1H, d), 5.04 (2H, s), 4.70 (2H, s),3.12-3.06 (4H, m), 2.55 (2H, t), 2.32 (2H, t).

Example 2961-(4-Fluorobenzyl)-4-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)pyridin-2(1H)-one

was prepared as described in EXAMPLE 295

¹H-NMR (DMSO-d₆) δ: 7.91 (2H, d), 7.73 (1H, d), 7.62 (2H, d), 7.35-7.34(2H, m), 7.17-7.13 (2H, m), 6.26 (1H, s), 6.13 (1H, dd), 5.03 (2H, s),4.83 (2H, s), 3.15-3.12 (4H, m), 2.65 (2H, t), 2.34 (2H, t).

Example 2974-(4-((1H-Benzo[d]imidazol-2-yl)methoxyimino)piperidin-1-ylsulfonyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 298 1-(3-Chlorophenylsulfonyl)piperidin-4-oneO-(1H-benzo[d]imidazol-2-yl)methyl oxime

was prepared as described in EXAMPLE 50

Example 2993-(4-((1H-Benzo[d]imidazol-2-yl)methoxyimino)piperidin-1-ylsulfonyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 300 1-(Quinolin-8-ylsulfonyl)piperidin-4-oneO-(1H-benzo[d]imidazol-2-yl)methyl oxime

was prepared as described in EXAMPLE 50

Example 301 1-(4-Fluorophenylsulfonyl)piperidin-4-oneO-(1H-benzo[d]imidazol-2-yl)methyl oxime

was prepared as described in EXAMPLE 50

Example 3023-(2-Morpholino-1-(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)ethyl)benzonitrile

was prepared as described in Example 107. Starting material was3-(1-(aminooxy)-2-morpholinoethyl)benzonitrile (see example A34).

¹H-NMR (DMSO-d₆) δ: 7.90 (2H, d), 7.70 (2H, d), 7.63-7.60 (3H, m), 7.50(1H, t), 5.23 (1H, t), 3.47 (4H, t), 3.16-3.01 (4H, m), 2.74-2.26 (10H,m).

Example 3033-(2-Isopropoxy-1-(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)ethyl)benzonitrile

was prepared as described in Example 107. Starting material was3-(1-(aminooxy)-2-isopropoxyethyl)benzonitrile (see example A35).

¹H-NMR (DMSO-d₆) δ: 7.91 (2H, d), 7.72-7.71 (2H, m), 7.64-7.62 (3H, m),7.51 (1H, t), 5.14 (1H, t), 3.67-3.46 (3H, m), 3.11-3.08 (4H, m), 2.69(2H, t), 2.30 (2H, t), 0.98 (6H, d).

Example 3043-(2-(4-Fluorophenoxy)-1-(1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)ethyl)benzonitrile

was prepared as described in Example 107. Starting material was3-(1-(aminooxy)-2-(4-fluorophenoxy)ethyl)benzonitrile (see example A36).

¹H-NMR (DMSO-d₆) δ: 7.90 (2H, d), 7.84 (1H, s), 7.74 (2H, dd), 7.63 (2H,d), 7.55 (1H, t), 7.05 (2H, t), 6.93-6.91 (2H, m), 5.42 (1H, dd),4.27-4.21 (2H, m), 3.09-3.08 (4H, m), 2.68-2.66 (2H, m), 2.31-2.30 (2H,m).

Example 305 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(3H-imidazo[4,5-b]pyridin-2-yl)methyl oxime

To a solution of tert-butyl2-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)-3H-imidazo[4,5-b]pyridine-3-carboxylate(prepared as described in Example 107 starting from tert-butyl2-(aminooxymethyl)-3H-imidazo[4,5-b]pyridine-3-carboxylate (see exampleA37), 256 mg, 0.450 mmol) in dichloroethane (4 ml), trifluoroacetic acid(0.70 ml, 9.0 mmol) was added and stirred at room temperature for 1hour. The reaction mixture was quenched with ammonia solution at 0° C.,extracted with chloroform, dried (MgSO₄) and evaporated under reducedpressure. The residue was purified by column chromatography on silica(chloroform/methanol, 98/2-90/10) to give the title compound (110 mg,52%).

Example 306 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-cyclopropyl(4-fluorophenyl)methyl oxime

was prepared as described in Example 107. Starting material wasO-(cyclopropyl(4-fluorophenyl)methyl)hydroxylamine (see example A38).

¹H-NMR (DMSO-d₆) δ: 7.90 (2H, d), 7.63 (2H, d), 7.30 (2H, dd), 7.09 (2H,t), 4.38 (1H, d), 3.17-3.11 (2H, m), 3.04-3.01 (2H, m), 2.68-2.66 (2H,m), 2.27 (2H, dd), 1.14-1.09 (1H, m), 0.54 (1H, q), 0.43-0.30 (3H, m).

Example 307 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-cyclopropyl(3-(trifluoromethyl)phenyl)methyl oxime

was prepared as described in Example 107. Starting material wasO-(cyclopropyl(3-(trifluoromethyl)phenyl)methyl)hydroxylamine (seeexample A39).

¹H-NMR (DMSO-d₆) δ: 7.90 (2H, d), 7.61-7.53 (6H, m), 4.50 (1H, d),3.28-3.22 (2H, m), 2.89-2.79 (3H, m), 2.66-2.61 (1H, m), 2.30-2.23 (2H,m), 1.14-1.12 (1H, m), 0.58-0.57 (1H, m), 0.45-0.42 (3.1H, m).

Example 308 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(6-chloro-3H-imidazo[4,5-b]pyridin-2-yl)methyl oxime

was prepared as described in Example 305. Starting material wastert-butyl2-(aminooxymethyl)-6-chloro-3H-imidazo[4,5-b]pyridine-3-carboxylate (seeexample A40).

¹H-NMR (DMSO-d₆) δ: 8.32 (1H, d), 8.06 (1H, s), 7.91 (2H, d), 7.63 (2H,d), 5.19 (2H, s), 3.13 (4H, t), 2.69 (2H, t), 2.34 (2H, t).

Example 309 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-cyclohexyl oxime

was prepared as described in EXAMPLE 65

Example 310 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-phenethyl oxime

was prepared as described in EXAMPLE 65

Example 311 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-biphenyl-2-ylmethyl oxime

was prepared as described in Example 107.

¹H-NMR (CDCl₃) δ: 7.81 (2H, dd), 7.46-7.28 (11H, m), 4.97 (2H, s), 3.19(2H, t), 3.11 (2H, t), 2.65 (2H, t), 2.40 (2H, t).

Example 312 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-biphenyl-3-ylmethyl oxime

was prepared as described in Example 107.

Example 313 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(3-phenylpyridin-2-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((3-phenylpyridin-2-yl)methyl)hydroxylamine (see example A41).

¹H-NMR (CDCl₃) δ: 8.62 (1H, d), 7.81 (2H, d), 7.63 (1H, d), 7.35-7.33(8H, m), 5.12 (2H, s), 3.17 (2H, t), 3.09 (2H, t), 2.59 (2H, t), 2.38(2H, t).

Example 3141-(4-Fluorophenyl)-5-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)pyridin-2(1H)-one

To a suspension of5-[1-(4-Trifluoromethoxybenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one(223 mg, 0.500 mmol), K₂CO₃ (138 mg, 1.00 mmol) and CuI (19 mg, 0.10mmol) in toluene (2 ml), a solution of p-bromofluorobenzene (0.060 ml,0.600 mmol) and (1S,2S)-(+)-N,N′-dimethylcyclohexane 1,2-diamine (14 mg,0.100 mmol) was added and refluxed for 19 hours. The solvent wasevaporated under reduced pressure and the residue was purified by columnchromatography on silica (ethyl acetate/hexane, 50/50-70/30) to give thetitle compound (241 mg, 89%).

¹H-NMR (DMSO-d₆) δ: 7.90 (2H, d), 7.67-7.62 (3H, m), 7.49-7.46 (3H, m),7.33 (2H, t), 6.47 (1H, d), 4.75 (2H, s), 3.15-3.08 (4H, m), 2.58 (2H,t), 2.36 (2H, t).

Example 3154-(2-oxo-5-((1-(4-(trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)pyridin-1(2H)-yl)benzonitrile

was prepared as described in Example 314.

¹H-NMR (DMSO-d₆) δ: 8.00 (2H, d), 7.90 (2H, d), 7.73 (1H, d), 7.65-7.62(4H, m), 7.53 (1H, dd), 6.50 (1H, d), 4.76 (2H, s), 3.15-3.08 (4H, m),2.58 (2H, t), 2.35 (2H, t).

Example 3161-(4-(4-(3-(Trifluoromethyl)benzyloxyimino)piperidin-1-ylsulfonyl)phenyl)ethanone

was prepared as described in EXAMPLE 50

Example 3173-((1-(4-Acetylphenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)benzonitrile

was prepared as described in EXAMPLE 50

Example 3181-(4-(4-(4-Chlorobenzyloxyimino)piperidin-1-ylsulfonyl)phenyl)ethanone

was prepared as described in EXAMPLE 50

Example 319 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-3-(trifluoromethyl)phenyl oxime

was prepared as described in Example 107.

Example 320 1-(6-benzylaminopyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

To a solution of 1-(6-chloropyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (134 mg, 0.300 mmol) in tetrahydrofuran(3 ml), benzylamine (161 mg, 1.50 mmol) was added and stirred at 80° C.for 40 hours. The solvent was evaporated under reduced pressure and theresidue was diluted with ethyl acetate and washed with H₂O and brine,dried (MgSO4) and evaporated under reduced pressure. The residue waspurified by column chromatography on silica (ethyl acetate/hexane25/75-50/50) to give the title compound (151 mg, 97%).

Example 321 1-(6-Cyclopropylaminopyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 320

¹H-NMR (DMSO-d₆) δ: 8.30 (1H, d), 7.80 (1H, d), 7.68-7.59 (5H, m), 6.67(1H, t), 5.09 (2H, s), 3.04-3.00 (4H, m), 2.64-2.63 (3H, m), 2.33 (2H,t), 0.76-0.74 (2H, m), 0.49-0.46 (2H, m).

Example 322 1-(6-Phenylaminopyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

A solution of 1-(6-chloropyridine-3-sulfonyl)piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime (134 mg, 0.300 mmol), aniline (0.027ml, 0.300 mmol), palladium (II) acetate (2.0 mg, 0.009 mmol),4,5-bis(diphenylphosphino)-9,9-dimethylxanthene (10 mg, 0.018 mmol) andsodium tert-butoxide (40 mg, 0.42 mmol) in dioxane (3 ml) was stirred at100° C. for 30 minutes. The solvent was evaporated under reducedpressure and the residue was diluted with ethyl acetate and washed withH₂O and brine, dried (MgSO₄) and evaporated under reduced pressure. Theresidue was purified by column chromatography on silica (ethylacetate/hexane 20/80-100/0) to give the title compound (43 mg, 28%).

Example 3236-[1-(4-Butylbenzenesulfonyl)piperidin-4-ylideneaminooxymethyl]-1H-pyridin-2-one

To a solution of 1-(4-butylbenzenesulfonyl)piperidin-4-oneO-(6-methoxypyridin-2-ylmethyl)oxime (60 mg, 0.139 mmol) and KI (115 mg,0.695 mmol) in acetonitrile (2 ml), chlorotrimethylsilane (76 mg, 0.695mmol) was added and stirred at room temperature for 5 hours and at 65°C. for 1 hour. 10% aqueous Na₂S₂O₃ solution (20 ml) was added, extractedwith ethyl acetate (30 ml×2), washed with brine, dried (MgSO₄) andevaporated under reduced pressure. The residue was purified by columnchromatography on silica (ethyl acetate/methanol, 100/0-90/10) to affordthe title compound (50 mg, 86%).

Example 324 1-[2-(2-Methoxy-ethoxy)benzenesulfonyl]piperidin-4-oneO-(3-trifluoromethylbenzyl)oxime

was prepared as described in EXAMPLE 91

Example 3252-(Piperidin-1-yl)-1-(4-(3-(trifluoromethyl)benzyloxyimino)piperidin-1-yl)ethanone

a) Chloroacetyl chloride (0.55 g, 5.0 mmol) was added to a mixture ofpiperidin-4-one O-3-(trifluoromethyl)benzyl oxime (1.0 g, 3.6 mmol) andtriethylamine in dichloromethane (20 ml) at 0° C. The reaction mixturewas warmed to room temperature over 6 h, washed with H₂O (10 ml) andevaporated under reduced pressure. The residue was purified by columnchromatography on silica to afford2-chloro-1-(4-(3-(trifluoromethyl)benzyloxyimino)piperidin-1-yl)ethanone(1.0 g, 70%).

b) A mixture of2-chloro-1-(4-(3-(trifluoromethyl)benzyloxyimino)piperidin-1-yl)ethanone(0.25 g, 0.70 mmol), K₂CO₃ (1.0 g, 7.8 mmol), KI (20 mg) and piperidine(0.07 ml, 0.8 mmol) in acetonitrile (4 ml) was stirred at 40° C. for 48hours. After cooling to room temperature, the reaction mixture wasdiluted with ethyl acetate (10 ml), washed with H₂O and evaporated underreduced pressure. The residue was purified by column chromatography onsilica (ethyl acetate/hexane, 30/70) to afford the title compound (100mg, 36%).

¹H-NMR (CDCl₃) δ: 7.45-7.60 (4H, m), 5.12 (2H, d), 3.64-3.72 (4H, m),3.16 (2H, s), 2.69-2.73 (1H, m), 2.61-2.64 (1H, m), 2.33-2.44 (6H, m),1.54-1.59 (4H, m), 1.40-1.45 (2H, m).

Example 3262-(2,2,2-Trifluoroethylamino)-1-(4-(3-(trifluoromethyl)benzyloxyimino)piperidin-1-yl)ethanone

was prepared as described in EXAMPLE 325

Example 327N-(3,5-Bis(trifluoromethyl)phenyl)-2-(4-(3-(trifluoromethyl)benzyloxyimino)piperidin-1-yl)acetamide

a) Chloroacetyl chloride (1.2 g) was added to a solution of3,5-bis(trifluoromethyl)aniline (2.0 g) and triethylamine (2 ml) indichloromethane (20 ml) at at 0° C. The reaction mixture was warmed toroom temperature over 3 hours, quenched with H₂O (6 ml), washed withbrine (4 ml) and evaporated under reduced pressure. The residue waspurified by column chromatography on silica (ethyl acetate/hexane,10/90) to afford N-(3,5-bis(trifluoromethyl)phenyl)-2-chloroacetamide ascolorless oil.

b) A mixture of N-(3,5-bis(trifluoromethyl)phenyl)-2-chloroacetamide(150 mg), piperidin-4-one O-3-(trifluoromethyl)benzyl oxime (120 mg),K₂CO₃ (300 mg), and KI (20 mg) in acetonitrile (4 ml) was stirred at 40°C. for 72 hours. The reaction mixture was diluted with ethyl acetate (4ml), washed with H₂O (2 ml), brine (4 ml) and evaporated under reducedpressure. The residue was purified by column chromatography on silica(ethyl acetate/hexane, 30/70) to afford the title compound (140 mg,50%).

¹H-NMR (CDCl₃) δ: 9.40 (1H, br), 8.08 (2H, s), 7.45-7.65 (5H, m), 5.12(2H, s), 3.64-3.72 (4H, m), 3.24 (2H, s), 2.71-2.83 (6H, m), 2.44-2.49(2H, m).

Example 3282-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-yl)-N-(3,5-bis(trifluoromethyl)phenyl)acetamide

was prepared as described in EXAMPLE 327

Example 329N-(3,5-Bis(trifluoromethyl)benzyl)-2-(4-(3-(trifluoromethyl)benzyloxyimino)piperidin-1-yl)acetamide

was prepared as described in EXAMPLE 327

Example 3302-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-yl)-N-(3,5-bis(trifluoromethyl)benzyl)acetamide

was prepared as described in EXAMPLE 327

Example 331N-(2-Ethoxy-4-fluorophenyl)-2-(4-(3-(trifluoromethyl)benzyloxyimino)piperidin-1-yl)acetamide

was prepared as described in EXAMPLE 327

Example 3322-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-yl)-N-(2-ethoxy-4-fluorophenyl)acetamide

was prepared as described in EXAMPLE 327

Example 333 1-(4-Butylphenylsulfonyl)piperidin-4-oneO-4-chloro-2-fluorobenzyl oxime

was prepared as described in EXAMPLE 65

Example 3342-((1-(3-Chlorophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107.

Example 3352-((1-(Pyridin-3-ylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107.

Example 336 1-(3-Fluorophenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in Example 107.

Example 3373-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-ylsulfonyl)-N-methoxy-N-methylbenzamide

was prepared as described in Example 107.

Example 3383-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-ylsulfonyl)-N,N-dimethylbenzamide

was prepared as described in Example 107.

Example 339 1-(Pyridin-3-ylsulfonyl)piperidin-4-one O-4-chlorobenzyloxime

was prepared as described in Example 107.

Example 3402-((1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107.

Example 3412-((1-(3-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107.

Example 342 1-(Pyridin-2-ylsulfonyl)piperidin-4-one O-4-chlorobenzyloxime

was prepared as described in Example 107.

Example 343 1-(3-Chlorophenylsulfonyl)piperidin-4-one O-4-chlorobenzyloxime

was prepared as described in Example 107.

Example 344 1-(Quinolin-8-ylsulfonyl)piperidin-4-one O-4-chlorobenzyloxime

was prepared as described in Example 107.

Example 3452-((1-(4-Chlorophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107.

Example 346 1-(4-Fluorophenylsulfonyl)piperidin-4-one O-4-chlorobenzyloxime

was prepared as described in Example 107.

Example 347 1-(3-Fluorophenylsulfonyl)piperidin-4-one O-4-chlorobenzyloxime

was prepared as described in Example 107.

Example 3482-((1-(4-Cyanophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107.

Example 3492-((1-(3-Cyanophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107.

Example 350 1-(4-Chlorophenylsulfonyl)piperidin-4-oneO-bis(4-fluorophenyl)methyl oxime

was prepared as described in Example 107.

Example 351 1-(4-Chlorophenylsulfonyl)piperidin-4-one O-4-chlorobenzyloxime

was prepared as described in Example 107.

Example 3522-((1-(4-Fluorophenylsulfonyl)piperidin-4-ylideneaminooxymethyl)isonicotinonitrile

was prepared as described in Example 107.

Example 3532-((1-(3-Fluorophenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107.

Example 3542-((1-(2-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107.

Example 3552-((1-(Quinolin-8-ylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107.

Example 3562-((1-(Pyridin-2-ylsulfonyl)piperidin-4-ylideneaminooxy)methyl)isonicotinonitrile

was prepared as described in Example 107.

Example 357 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(6-chloropyridin-3-yl)methyl oxime

was prepared as described in Example 107.

Example 358 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(2-chloropyridin-3-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((2-chloropyridin-3-yl)methyl)hydroxylamine (see example A42).

Example 359 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-4-chlorobenzyl oxime

was prepared as described in Example 107.

Example 360 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-propyl oxime

was prepared as described in EXAMPLE 65

Example 361 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-isobutyl oxime

was prepared as described in EXAMPLE 65

Example 362 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-isopropyl oxime

was prepared as described in EXAMPLE 65

Example 363 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-isobutyl oxime

was prepared as described in EXAMPLE 65

Example 364 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-3-methylbut-2-enyl oxime

was prepared as described in EXAMPLE 65

Example 365 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-propyl oxime

was prepared as described in EXAMPLE 65

Example 366 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-isopentyl oxime

was prepared as described in EXAMPLE 65

¹H-NMR (CDCl₃) δ: 8.03 (1H, s), 7.96 (1H, d), 7.87 (1H, d), 7.70 (1H,dd), 4.0 (2H, t), 3.24 (2H, t), 3.17 (2H, t), 2.7 (2H, t), 2.45 (2H,dd), 1.60-1.68 (1H, m), 1.46-1.51 (2H, m), 0.89 (6H, d).

Example 367 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-hexan-2-yl oxime

was prepared as described in EXAMPLE 65

¹H-NMR (CDCl₃) δ: 8.03 (1H, s), 7.96 (1H, d), 7.87 (1H, d), 7.70 (1H,dd), 4.04-4.09 (1H, m), 3.24 (2H, t), 3.17 (2H, t), 2.70 (2H, t), 2.45(2H, dd), 1.20-1.60 (6H, m), 1.15 (3H, d), 0.87-0.90 (3H, m).

Example 368 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-cinnamyl oxime

was prepared as described in EXAMPLE 65

¹H-NMR (CDCl₃) δ: 8.03 (1H, s), 7.96 (1H, d), 7.87 (1H, d), 7.70 (1H,dd), 7.28-7.38 (5H, m), 6.58 (1H, d), 6.30 (1H, dt), 4.64 (2H, dd), 3.25(2H, t), 3.18 (2H, t), 2.74 (2H, dd), 2.47 (2H, dd).

Example 369 1-(3-(Trifluoromethyl)phenylsulfonyl)piperidin-4-oneO-heptan-2-yl oxime

was prepared as described in EXAMPLE 65

¹H-NMR (CDCl₃) δ: 8.03 (1H, s), 7.96 (1H, d), 7.87 (1H, d), 7.70 (1H,dd), 4.04-4.09 (1H, m), 3.23 (2H, t), 3.16 (2H, t), 2.70 (2H, t), 2.45(2H, t), 1.20-1.60 (8H, m), 1.14 (3H, d), 0.84-0.87 (3H, m).

Example 3703-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-ylsulfonyl)-N-methylbenzamide

was prepared as described in Example 107.

Example 3713-(4-(Bis(4-fluorophenyl)methoxyimino)piperidin-1-ylsulfonyl)benzamide

was prepared as described in Example 107.

Example 372 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(3-chloropyridin-4-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((3-chloropyridin-4-yl)methyl)hydroxylamine (see example A43).

Example 373 1-(4-(Ttrifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(6-chloropyridin-2-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((6-Chloropyridin-2-yl)methyl)hydroxylamine (see example A44).

Example 374 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(4-chloropyridin-3-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((4-Chloropyridin-3-yl)methyl)hydroxylamine (see example A45).

Example 375 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(2-chloropyridin-4-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((2-Chloropyridin-4-yl)methyl)hydroxylamine (see example A46).

Example 376 1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-oneO-(3-chloropyridin-2-yl)methyl oxime

was prepared as described in Example 107. Starting material wasO-((3-Chloropyridin-2-yl)methyl)hydroxylamine (see example A47).

Example 3775-((1-(4-(Trifluoromethoxy)phenylsulfonyl)piperidin-4-ylideneaminooxy)methyl)nicotinonitrile

was prepared as described in Example 107. Starting material was5-(Aminooxymethyl)nicotinonitrile (see example A48).

Purity of compounds was verified by LCMS measurement. LCMS method is asfollows;

Method A

Column: Phenomemex Luna C18 (4.6×50 mm, 5 micron particle size),Temperature: 50° C., Monitored at OD 254 nm, reference 360 nm, Flowrate: 2 ml/min.

HPLC Gradient (Buffer A=0.1% formic acid/H₂O, Buffer B=0.1% formicacid/acetonitrile)

TABLE 2 Time (min.) % B 0 15 1.9 45 4.3 45 8.3 95 11.3 95 11.4 15 15.415

Method B

Column: Discovery HS C18 (4.6×150 mm, 3 micron particle size),Temperature: 25° C., Monitored at OD 260 nm, reference 360 nm, Flowrate: 1 ml/min.

HPLC Gradient (Buffer A=0.1% trifluoroacetic acid/H₂O, Buffer B=0.1%trifluoroacetic acid/acetonitrile)

TABLE 3 Time (min.) % B 0 15 1.9 45 4.3 45 8.3 95 11.3 95 11.4 15 15.415

Method C

Column: Sunfire-C18 (2.1×50 mm, 3.5 micron particle size), Temperature:50° C., Monitored at OD 214 nm, reference 360 nm, Flow rate: 0.9 ml/min.

HPLC Gradient (Buffer A=0.05% trifluoroacetic acid/H₂O, Buffer B=0.05%trifluoroacetic acid/acetonitrile)

TABLE 4 Time (min.) % B 0 10 2.2 90 4.0 90

TABLE 5 LCMS data and properties of the example compounds EXAMPLE LCMSRetention Purity Compound Method time (min) (%) M/Z Form 1 A 2.60 100399 colorless solid 2 A 2.35 100 331 colorless solid 3 A 2.58 100 399colorless solid 4 A 2.45 96 365 colorless solid 5 A 0.68 100 332 yellowsolid 6 A 1.17 100 332 colorless solid 7 A 1.83 100 366 colorless solid8 A 2.55 98 385 colorless solid 9 A 2.34 100 365 colorless solid 10 A1.93 100 356 colorless solid 11 A 2.51 100 399 colorless solid 12 A 3.40100 516 colorless solid 13 A 3.28 100 482 colorless solid 14 A 3.14 99434 colorless solid 15 A 3.26 98 462 colorless solid 16 A 2.17 100 449colorless solid 17 A 1.93 100 449 off-white solid 18 A 3.87 100 463colorless solid 19 A 3.24 100 463 yellow solid 20 A 6.96 100 376colorless oil 21 A 7.36 100 404 colorless oil 22 A 7.13 100 419colorless oil 23 A 6.85 100 391 colorless solid 24 A 2.58 100 399colorless solid 25 A 2.50 100 419 off-white solid 26 A 2.02 100 317off-white solid 27 A 2.13 98 331 tan solid 28 A 2.10 97 351 colorlesssolid 29 A 8.36 100 530 colorless oil 30 A 8.31 100 530 colorless oil 31A 7.90 100 462 colorless oil 32 A 3.07 100 448 colorless solid 33 A 3.53100 516 colorless solid 34 A 2.45 100 399 colorless solid 35 A 2.09 100427 colorless amorphous 36 A 2.18 100 441 tan solid 37 A 2.16 100 387colorless oil 38 A 2.08 99 401 colorless oil 39 A 2.19 100 401 colorlessoil 40 A 2.02 100 456 tan solid 41 A 2.08 100 413 tan solid 42 A 2.54100 503 colorless solid 43 A 2.02 96 426 tan solid 44 A 2.63 100 488 tansolid 45 A 2.23 98 454 off-white solid 46 A 1.99 98 456 off-white solid47 A 2.70 100 487 off-white solid 48 A 2.85 100 501 tan solid 49 A 2.74100 449 ale-yellow solid 50 A 8.82 100 468 colorless solid 51 A 7.68 100412 colorless solid 52 A 6.13 100 350 colorless solid 53 A 7.37 100 437colorless solid 54 A 5.42 97 416 pale-yellow oil 55 A 8.54 100 480colorless solid 56 A 8.46 100 480 pale-yellow solid 57 A 8.39 100 480yellow solid 58 A 8.54 100 496 colorless solid 59 A 8.57 100 496pale-yellow solid 60 A 8.58 100 496 colorless oil 61 A 8.39 100 442colorless solid 62 A 7.88 100 430 colorless solid 63 A 8.33 97 430colorless solid 64 A 8.21 100 447 colorless solid 65 A 9.16 100 434pale-yellow solid 66 A 8.89 100 468 colorless solid 67 A 8.50 100 400colorless solid 68 A 6.21 100 401 pale-yellow solid 69 A 8.19 100 435pale-yellow solid 70 A 5.57 100 401 colorless solid 71 A 4.13 100 401pale-yellow solid 72 A 9.06 100 434 colorless solid 73 A 8.39 97 435colorless solid 74 A 9.29 100 482 colorless solid 75 A 8.62 100 435pale-yellow solid 76 A 8.65 100 431 colorless solid 77 A 9.21 100 425colorless solid 78 A 8.31 100 468 pale-yellow oil 79 A 9.19 100 484pale-yellow solid 80 A 8.69 100 430 pale-yellow solid 81 A 9.21 100 486pale-yellow oil 82 A 10.08 97 406 pale-yellow solid 83 A 6.61 100 427off-white solid 84 A 6.95 100 427 colorless solid 85 A 7.40 100 427colorless solid 86 A 6.21 100 471 yellow solid 87 A 6.57 98 471pale-yellow oil 88 A 6.57 98 471 colorless oil 89 A 2.67 100 484colorless solid 90 A 2.74 100 470 yellow solid 91 A 8.84 100 456 yellowsolid 92 A 9.15 100 470 pale-yellow solid 93 A 8.64 97 470 colorlesssolid 94 A 8.13 98 486 pale-yellow solid 95 A 8.87 100 482 pale-yellowsolid 96 A 7.27 100 456 colorless solid 97 A 7.60 100 482 pale-yellowsolid 98 A 7.21 100 498 colorless solid 99 A 7.40 100 470 pale-yellowsolid 100 A 7.61 100 443 colorless solid 101 A 8.19 100 505 colorlesssolid 102 A 8.42 100 519 colorless solid 103 A 8.37 100 471 colorlesssolid 104 A 8.31 100 489 pale-yellow solid 105 A 4.76 98 429 colorlesssolid 106 A 5.93 100 441 pale-yellow solid 107 A 6.05 98 429 pale-yellowsolid 108 A 8.42 100 471 colorless solid 109 A 9.05 100 462 colorlesssolid 110 A 8.46 100 459 colorless solid 111 A 8.49 100 459 colorlesssolid 112 A 5.75 100 445 colorless solid 113 A 5.64 100 445 colorlesssolid 114 A 8.46 95 436 colorless solid 115 A 9.68 95 434 colorlesssolid 116 A 9.45 100 420 colorless solid 117 A 7.13 100 430 pale-yellowsolid 118 A 8.26 100 463 colorless solid 119 A 9.29 100 540 colorlessamorphous 120 A 8.40 97 453 colorless solid 121 A 8.32 100 453 colorlesssolid 122 A 8.26 100 453 colorless solid 123 A 8.73 100 446 colorlesssolid 124 A 8.01 100 443 colorless solid 125 A 7.96 100 447 colorlesssolid 126 A 7.81 100 447 colorless solid 127 A 8.43 100 463 colorlesssolid 128 A 8.43 100 471 colorless solid 129 A 9.44 100 476 colorlesssolid 130 A 3.07 100 435 colorless solid 131 A 3.08 100 449 colorlesssolid 132 A 7.43 100 477 colorless oil 133 A 7.16 95 443 colorless solid134 A 8.71 100 473 colorless solid 135 A 6.97 100 443 pale-yellow solid136 A 3.07 100 435 colorless solid 137 A 3.06 98 449 colorless solid 138A 7.21 100 477 colorless solid 139 A 8.17 100 436 colorless solid 140 A6.65 100 459 pale-yellow solid 141 A 6.77 100 459 pale-yellow solid 142A 3.04 100 432 pale-yellow solid 143 A 9.35 100 468 colorless solid 144A 8.42 100 459 colorless solid 145 A 5.46 100 445 colorless solid 146 A6.38 100 459 pale-yellow solid 147 A 9.14 95 493 colorless solid 148 A8.46 100 459 colorless solid 149 A 7.63 100 479 colorless solid 150 A5.69 100 445 colorless solid 151 A 6.50 100 459 colorless solid 152 A7.71 100 493 colorless solid 153 A 6.33 100 383 pale-yellow oil 154 A6.71 100 397 colorless solid 155 A 6.72 96 395 colorless solid 156 A6.39 100 399 colorless solid 157 A 5.89 100 398 colorless solid 158 A7.20 100 385 pale-yellow oil 159 A 4.75 100 366 pale-yellow solid 160 A3.51 100 482 colorless solid 161 A 2.44 100 432 pale-yellow solid 162 A3.14 100 468 colorless solid 163 A 7.71 96 489 colorless solid 164 A7.64 100 491 colorless solid 165 A 5.77 100 443 colorless solid 166 A6.43 100 398 pale-yellow solid 167 A 2.91 100 398 pinkish solid 168 A5.54 100 402 pale-yellow solid 169 A 7.53 100 442 pale-yellow solid 170A 8.05 100 507 pale-yellow solid 171 A 5.21 97 444 yellow solid 172 A6.38 100 435 colorless solid 173 A 7.20 100 454 colorless solid 174 A2.44 100 437 colorless solid 175 A 2.40 100 437 colorless solid 176 A6.52 100 416 yellow solid 177 A 7.14 100 454 pale-yellow solid 178 A6.96 100 454 colorless solid 179 A 2.84 100 459 colorless solid 180 A7.69 100 492 pale-yellow solid 181 A 7.83 100 505 colorless oil 182 A7.77 97 449 pale-yellow solid 183 A 7.45 100 492 pale-yellow solid 184 A6.98 100 465 colorless solid 185 A 8.87 95 482 colorless solid 186 A8.08 100 493 colorless oil 187 A 4.19 98 500 colorless solid 188 A 2.32100 442 pale-yellow solid 189 A 3.83 95 509 yellow solid 190 A 8.34 97553 colorless amorphous 191 A 6.58 100 483 colorless amorphous 192 A8.03 100 503 colorless solid 193 A 4.79 100 495 colorless solid 194 A3.01 100 445 light-green solid 195 A 8.55 100 504 colorless amorphous196 B 10.11 100 387 colorless solid 197 B 10.17 100 435 colorless solid198 B 10.05 100 399 colorless solid 199 B 9.89 99 394 colorless solid200 A 8.24 100 489 colorless solid 201 A 7.20 100 438 colorless solid202 A 7.25 97 436 pale-yellow solid 203 A 3.16 100 512 colorless solid204 A 7.72 100 467 colorless solid 205 B 9.81 100 429 colorless solid206 B 9.99 100 429 colorless solid 207 B 10.02 100 412 colorless solid208 B 10.33 99 405 colorless solid 209 B 10.20 100 405 colorless solid210 B 10.29 97 405 colorless solid 211 B 10.24 98 405 colorless solid212 A 7.98 100 486 colorless solid 213 A 6.78 100 472 colorless solid214 A 6.48 95 539 colorless solid 215 A 3.10 96 526 colorless solid 216A 2.98 100 529 pale-yellow solid 217 A 7.50 98 467 light-red solid 218 B9.82 100 442 colorless solid 219 B 9.91 99 443 colorless solid 220 B9.09 100 428 colorless solid 221 B 9.15 99 429 colorless solid 222 B10.49 99 438 colorless solid 223 B 9.74 100 456 colorless solid 224 B11.33 100 527 colorless solid 225 B 11.41 100 571 colorless solid 226 B10.09 100 469 colorless solid 227 B 10.34 100 513 colorless oil 228 B11.31 95 525 colorless solid 229 B 10.62 96 481 colorless solid 230 B11.15 93 470 colorless solid 231 B 11.62 97 512 colorless solid 232 B10.97 96 522 colorless solid 233 B 10.84 95 522 colorless solid 234 B10.83 96 509 pale-yellow solid 235 B 10.78 97 522 colorless solid 236 B10.69 97 500 colorless solid 237 B 10.90 95 527 colorless solid 238 B10.74 96 486 colorless solid 239 A 5.86 100 471 colorless solid 240 A6.61 100 485 colorless solid 241 A 6.76 100 499 colorless solid 242 B10.90 100 475 colorless solid 243 B 11.09 95 492 colorless solid 244 B11.11 98 492 colorless solid 245 B 11.03 100 492 colorless solid 246 B10.93 100 474 colorless solid 247 B 11.92 100 452 colorless solid 248 B11.40 100 364 colorless solid 249 B 10.85 100 392 colorless solid 250 B10.65 100 376 colorless solid 251 B 9.76 100 507 colorless solid 252 B10.91 97 462 colorless solid 253 B 9.54 99 423 colorless solid 254 B8.78 100 460 colorless solid 255 B 9.46 100 420 colorless solid 256 B9.77 100 481 colorless solid 257 B 9.85 100 499 colorless solid 258 B9.92 100 516 colorless solid 259 B 11.03 98 492 colorless solid 260 B9.96 98 486 colorless solid 261 B 9.89 100 514 colorless solid 262 B8.48 100 474 colorless solid 263 A 7.28 100 469 pale-yellow solid 264 A2.92 100 468 colorless solid 265 A 7.75 100 472 colorless solid 266 A4.38 98 486 colorless solid 267 B 9.76 100 481 colorless solid 268 B9.72 100 516 colorless solid 269 A 6.72 100 530 colorless solid 270 A5.65 98 530 colorless solid 271 A 7.54 100 530 colorless amorphous 272 A7.40 100 444 colorless solid 273 A 7.72 100 497 colorless oil 274 A 6.60100 465 pale-yellow amorhous 275 A 7.74 100 493 orange amorhous 276 B10.17 100 426 colorless oil 277 B 10.91 100 418 colorless solid 278 A7.26 100 435 colorless solid 279 B 9.96 100 413 colorless solid 280 B9.60 100 437 colorless solid 281 B 8.89 100 431 colorless solid 282 B8.75 100 394 colorless solid 283 B 8.58 98 420 colorless solid 284 B9.62 98 437 colorless solid 285 B 10.44 100 524 colorless oil 286 B10.08 100 514 colorless solid 287 B 9.93 100 462 colorless solid 288 B9.65 100 457 colorless solid 289 B 10.47 100 540 colorless oil 290 B10.52 98 540 colorless oil 291 B 9.40 100 457 colorless solid 292 B10.41 100 490 colorless solid 293 B 8.55 97 438 pale-yellow solid 294 B11.21 100 432 colorless solid 295 A 7.14 100 553 colorless solid 296 A7.18 100 553 colorless solid 297 B 5.27 99 409 colorless solid 298 B5.97 100 418 colorless solid 299 B 5.25 100 409 colorless solid 300 B5.02 100 435 colorless solid 301 B 5.39 100 402 colorless solid 302 A3.14 100 552 colorless amorphous 303 A 8.27 100 525 colorless oil 304 A8.39 100 577 colorless amorphous 305 A 4.33 100 469 colorless solid 306A 9.51 100 486 colorless oil 307 A 8.75 100 536 colorless solid 308 A6.47 100 503 pale-yellow solid 309 B 10.58 100 404 colorless solid 310 B3.35 100 426 colorless solid 311 A 8.06 100 504 colorless oil 312 A 7.86100 504 colorless solid 313 A 6.27 99 505 colorless oil 314 A 5.49 100539 colorless solid 315 A 5.09 100 546 colorless solid 316 A 6.69 98 454colorless solid 317 A 4.87 100 411 pale-yellow solid 318 A 6.57 100 420pale-yellow solid 319 A 7.78 100 482 colorless solid 320 A 8.37 100 518pale-yellow solid 321 A 7.67 100 468 yellow solid 322 A 8.49 97 504pale-yellow solid 323 A 6.77 97 417 pale-yellow solid 324 A 8.28 98 486pale-yellow oil 325 B 8.66 100 397 colorless solid 326 B 8.70 97 411colorless oil 327 B 10.01 100 541 colorless oil 328 B 10.18 100 585colorless oil 329 B 9.97 100 555 colorless oil 330 B 10.13 100 599colorless oil 331 B 9.61 95 467 colorless oil 332 B 9.75 100 511pale-yellow solid 333 B 11.95 100 452 colorless solid 334 C 2.75 100 404colorless solid 335 C 2.26 100 371 off-white solid 336 C 2.17 100 474colorless solid 337 C 2.98 100 543 off-white solid 338 C 2.92 100 527off-white solid 339 C 2.76 100 379 off-white solid 340 C 2.80 100 438off-white solid 341 C 2.84 100 454 off-white solid 342 C 2.84 100 379off-white solid 343 C 3.17 100 413 colorless solid 344 C 2.09 100 429colorless solid 345 C 2.72 100 404 colorless solid 346 C 3.06 100 396colorless solid 347 C 2.23 100 396 colorless solid 348 C 2.54 100 395off-white solid 349 C 2.53 100 395 off-white solid 350 C 3.24 100 490colorless solid 351 C 3.17 100 413 colorless solid 352 C 2.62 100 388colorless solid 353 C 2.64 100 388 colorless solid 354 C 2.79 100 454off-white solid 355 C 2.49 100 421 off-white solid 356 C 2.33 100 371off-white solid 357 C 2.97 100 463 off-white solid 358 C 2.96 100 463off-white solid 359 C 3.19 100 446 colorless solid 360 B 10.91 100 380colorless solid 361 B 11.16 100 394 colorless solid 362 B 10.68 100 364colorless solid 363 B 10.97 100 378 colorless solid 364 B 10.93 100 390colorless solid 365 B 10.73 98 364 colorless solid 366 B 10.46 100 392colorless solid 367 B 10.85 100 406 colorless oil 368 B 10.25 100 438colorless solid 369 B 11.15 100 420 colorless oil 370 C 2.88 99 513off-white solid 371 C 2.81 100 499 off-white solid 372 C 2.87 100 463off-white solid 373 C 3.01 100 463 pale-yellow solid 374 C 2.68 99 463off-white solid 375 C 2.97 100 463 off-white solid 376 C 2.88 98 463off-white solid 377 C 2.83 100 454 off-white solid

Compounds of the invention have been tested in the calcium mobilizationand/or electrophysiological assay for N-type calcium channel blockingactivity, which are described in detail above. Some compounds describedhave also been tested in the calcium mobilization assay for L-typecalcium channel blocking activity, which is described in detail above.Representative values are presented in TABLE 6.

TABLE 6 Evaluation of the tested compounds as N-type calcium channel(NTCC) blockers and L-type calcium channel (LTCC) blockers after acalcium mobilization in vitro assay EXAMPLE NTCC IC₅₀(nM) LTCC IC₅₀(nM)4 860 15200 8 690 9600 12 820 >20000 16 260 6600 19 760 4900 24 990 720050 430 >20000 30 330 >20000 77 220 >20000 182 690 >20000 227 1100 Notdetermined 277 610 >20000 295 160 >20000 308 360 >20000 328 1100 Notdetermined 369 80 >20000

The following compounds also exhibited an NTCC IC₅₀ of about 1.0 μM orless. 29, 31, 47, 48, 51, 53, 56, 58, 59, 62, 63, 64, 65, 67, 68, 69,70, 71, 72, 73, 74, 75, 76, 78, 79, 80, 81, 82, 85, 91, 93, 94, 95, 99,101, 108, 110, 111, 118, 119, 120, 121, 127, 128, 134, 144, 147, 152,160, 162, 163, 164, 173, 177, 178, 181, 186, 189, 191, 196, 197, 199,210, 214, 216, 228, 229, 231, 232, 237, 238, 243, 244, 251, 252, 256,263, 265, 267, 268, 269, 270, 271, 273, 274, 275, 276, 278, 280, 281,282, 284, 285, 286, 287, 288, 289, 290, 291, 292, 294, 296, 302, 303,304, 306, 307, 309, 310, 311, 313, 314, 315, 321, 329, 366, 367 and 368.

Having now fully described this invention, it will be understood bythose of ordinary skill in the art that the same can be performed withina wide and equivalent range of conditions, formulations and otherparameters without affecting the scope of the invention or anyembodiment thereof.

Other embodiments of the invention will be apparent to those skilled inthe art from consideration of the specification and practice of theinvention disclosed herein. It is intended that the specification andexamples be considered as exemplary only, with a true scope and spiritof the invention being indicated by the following claims. All patentsand publications cited herein are fully incorporated by reference hereinin their entirety.

1. A compound having the Formula I:

a pharmaceutically acceptable salt, a prodrug or a solvate thereof,wherein: W is absent, optionally substituted lower alkylene oroptionally substituted lower alkenylene, X is optionally substitutedaryl, optionally substituted heterocyclyl, optionally substitutedcycloalkyl or optionally substituted cycloalkenyl and When W isoptionally substituted lower alkylene or optionally substituted loweralkenylene, then X can additionally be hydrogen; Y is CO, SO_(m) orCR³R⁴; Z is optionally substituted lower alkyl, optionally substitutedlower alkenyl, optionally substituted lower alkynyl, optionallysubstituted lower alkoxy, optionally substituted lower alkenyloxy,optionally substituted lower alkynyloxy, optionally substituted amino,optionally substituted lower alkylthio, optionally substituted loweralkenylthio, optionally substituted lower alkynylthio, optionallysubstituted cycloalkyl, optionally substituted cycloalkenyl, optionallysubstituted aryl or optionally substituted heterocyclyl, when Y is CO,then Z can additionally be optionally substituted acyl, optionallysubstituted carbamoyl, optionally substituted cycloalkyloxy, optionallysubstituted cycloalkenyloxy, optionally substituted aryloxy oroptionally substituted heterocyclyloxy, when Y is CR³R⁴, then Z canadditionally be hydrogen, hydroxy, halogen, carboxy, optionallysubstituted lower alkoxycarbonyl, optionally substituted loweralkylthio, optionally substituted acyl, optionally substituted acyloxy,optionally substituted lower alkylsulfonyl, optionally substituted loweralkylsulfonyloxy, optionally substituted lower alkylsulfinyl, optionallysubstituted carbamoyl, optionally substituted carbamoyloxy, optionallysubstituted sulfamoyl, optionally substituted sulfamoyloxy, optionallysubstituted aryloxy, optionally substituted aryloxycarbonyl, optionallysubstituted arylthio, optionally substituted arylsulfonyl, optionallysubstituted arylsulfinyl, optionally substituted arylsulfonyloxy,optionally substituted arylsulfinyloxy, optionally substitutedheterocyclyloxy, optionally substituted heterocyclyloxycarbonyl,optionally substituted heterocyclylthio, optionally substitutedheterocyclylsulfonyl, optionally substituted heterocyclylsulfinyl,optionally substituted heterocyclylsulfonyloxy, optionally substitutedheterocyclylsulfinyloxy, R³ and R⁴ are each independently hydrogen,halogen, lower alkyl, halo(lower)alkyl, hydroxy(lower)alkyl, amino,lower alkylamino, optionally substituted cycloalkyl, optionallysubstituted cycloalkenyl, optionally substituted aryl or optionallysubstituted heterocyclyl, or together with the carbon atom to which theyare attached form optionally substituted carbocycle or optionallysubstituted heterocycle; R is lower alkyl, hydroxy(lower)alkyl, loweralkoxy(lower)alkyl, carboxy, lower alkoxycarbonyl, carbamoyl or loweralkylcarbamoyl, m is 1 or 2, p is 0, 1 or 2, and q is 0, 1 or 2 with thefollowing provisos: i) when Y is SO₂, then Z is not lower alkylsubstituted with at least one substituent selected from CONHOH, COOH andlower alkoxycarbonyl, ii) Y-Z is not benzoyl, acetyl, carbamoyl or loweralkoxycarbonyl, iii) when Y is CO, then Z is not methylene substitutedwith heterocyclidene, and iv) when Y is SO₂, then —W—X is not2-tetrahydrofuryl.
 2. The compound of claim 1, wherein q is
 1. 3. Thecompound of claim 1 or 2, wherein W is (CR¹R²)n, n is 0, 1, 2 or 3, R¹and R² are each independently hydrogen, halogen, lower alkyl,halo(lower)alkyl, hydroxy(lower)alkyl, lower alkoxy(lower)alkyl,optionally substituted aryl(lower)alkyl, optionally substitutedaryloxy(lower)alkyl, optionally substituted heterocyclyl(lower)alkyl,optionally substituted heterocyclyloxy(lower)alkyl, optionallysubstituted cycloalkyl, optionally substituted cycloalkenyl, optionallysubstituted aryl or optionally substituted heterocyclyl and X isoptionally substituted aryl, optionally substituted heterocyclyl,optionally substituted cycloalkyl or optionally substitutedcycloalkenyl.
 4. The compound of any of claims 1 to 3, wherein W isoptionally substituted methylene.
 5. The compound of any of claims 1 to4, wherein X is optionally substituted phenyl or optionally substitutedpyridyl.
 6. The compound of any of claims 1 to 5, wherein Y is CO orSO₂.
 7. The compound of any of claims 1 to 6, wherein Z is optionallysubstituted lower alkyl or optionally substituted phenyl.
 8. Apharmaceutical composition, comprising the compound of any of claims 1to 7 and a pharmaceutically acceptable carrier.
 9. A method of treating,preventing or ameliorating a disorder responsive to the blockade ofcalcium channels in a mammal suffering from said disorder, comprisingadministering to a mammal in need of such treatment, prevention oramelioration an effective amount of a compound of any of claims 1 to 7.10. The method of claim 9, wherein a disorder responsive to the blockadeof N-type calcium channels is treated, prevented or ameliorated.
 11. Amethod for treating, preventing or ameliorating stroke, neuronal damageresulting from head trauma, epilepsy, pain, migraine, a mood disorder,schizophrenia, a neurodegenerative disorder, depression, anxiety, apsychosis, hypertension or cardiac arrhythmia in a mammal, comprisingadministering an effective amount of a compound of any of claims 1 to 7.12. The method of claim 11, wherein the method is for treating,preventing or ameliorating pain selected from chronic pain, acute pain,and surgical pain.
 13. A method of modulating calcium channels in amammal, comprising administering to the mammal at least one compound ofany one of claims 1 to
 7. 14. The method of claim 13, wherein the N-typecalcium channel is modulated.
 15. A compound having the Formula I asclaimed in claims 1 to 7, wherein the compound is ³H, ¹¹C, or ¹⁴Cradiolabeled.
 16. A method of screening a candidate compound for theability to bind to a receptor using a radiolabeled compound of claim 15,comprising a) introducing a fixed concentration of the radiolabeledcompound to the receptor to form a mixture; b) titrating the mixturewith a candidate compound; and c) determining the binding of thecandidate compound to said receptor.
 17. Use of a compound of Formula Ias claimed in any one of claims 1 to 7 in the manufacture of amedicament for treating, preventing or ameliorating stroke, neuronaldamage resulting from head trauma, epilepsy, pain, migraine, a mooddisorder, schizophrenia, a neurodegenerative disorder, depression,anxiety, a psychosis, hypertension or cardiac arrhythmia in a mammal.18. Use of a compound of Formula I as claimed in any one of claims 1 to7 in the manufacture of a medicament for treating, preventing orameliorating pain selected from chronic pain, acute pain, and surgicalpain.
 19. A pharmaceutical composition for modulating calcium channelsin a mammal, comprising the compound having the Formula I′:

a pharmaceutically acceptable salt, a prodrug or a solvate thereof,wherein: W is absent, optionally substituted lower alkylene oroptionally substituted lower alkenylene, X is optionally substitutedaryl, optionally substituted heterocyclyl, optionally substitutedcycloalkyl or optionally substituted cycloalkenyl and When W isoptionally substituted lower alkylene or optionally substituted loweralkenylene, then X can additionally be hydrogen; Y is CO, SO_(m) orCR³R⁴; Z is optionally substituted lower alkyl, optionally substitutedlower alkenyl, optionally substituted lower alkynyl, optionallysubstituted lower alkoxy, optionally substituted lower alkenyloxy,optionally substituted lower alkynyloxy, optionally substituted amino,optionally substituted lower alkylthio, optionally substituted loweralkenylthio, optionally substituted lower alkynylthio, optionallysubstituted cycloalkyl, optionally substituted cycloalkenyl, optionallysubstituted aryl or optionally substituted heterocyclyl, when Y is CO,then Z can additionally be optionally substituted acyl, optionallysubstituted carbamoyl, optionally substituted cycloalkyloxy, optionallysubstituted cycloalkenyloxy, optionally substituted aryloxy oroptionally substituted heterocyclyloxy, when Y is CR³R⁴, then Z canadditionally be hydrogen, hydroxy, halogen, carboxy, optionallysubstituted lower alkoxycarbonyl, optionally substituted loweralkylthio, optionally substituted acyl, optionally substituted acyloxy,optionally substituted lower alkylsulfonyl, optionally substituted loweralkylsulfonyloxy, optionally substituted lower alkylsulfinyl, optionallysubstituted carbamoyl, optionally substituted carbamoyloxy, optionallysubstituted sulfamoyl, optionally substituted sulfamoyloxy, optionallysubstituted aryloxy, optionally substituted aryloxycarbonyl, optionallysubstituted arylthio, optionally substituted arylsulfonyl, optionallysubstituted arylsulfinyl, optionally substituted arylsulfonyloxy,optionally substituted arylsulfinyloxy, optionally substitutedheterocyclyloxy, optionally substituted heterocyclyloxycarbonyl,optionally substituted heterocyclylthio, optionally substitutedheterocyclylsulfonyl, optionally substituted heterocyclylsulfinyl,optionally substituted heterocyclylsulfonyloxy, optionally substitutedheterocyclylsulfinyloxy, when Z is optionally substituted cycloalkyl,optionally substituted cycloalkenyl, optionally substituted aryl oroptionally substituted heterocyclyl, then Y can additionally be absent;R³ and R⁴ are each independently hydrogen, halogen, lower alkyl,halo(lower)alkyl, hydroxy(lower)alkyl, amino, lower alkylamino,optionally substituted cycloalkyl, optionally substituted cycloalkenyl,optionally substituted aryl or optionally substituted heterocyclyl, ortogether with the carbon atom to which they are attached form optionallysubstituted carbocycle or optionally substituted heterocycle; R is loweralkyl, hydroxy(lower)alkyl, lower alkoxy(lower)alkyl, carboxy, loweralkoxycarbonyl, carbamoyl or lower alkylcarbamoyl, m is 1 or 2, p is 0,1 or 2, and q is 0, 1 or 2 and a pharmaceutically acceptable carrier.20. The pharmaceutical composition of claim 19, wherein q is
 1. 21. Thepharmaceutical composition of claim 19 or 20, wherein W is (CR¹R²)n, nis 0, 1, 2 or 3, R¹ and R² are each independently hydrogen, halogen,lower alkyl, halo(lower)alkyl, hydroxy(lower)alkyl, loweralkoxy(lower)alkyl, optionally substituted aryl(lower)alkyl, optionallysubstituted aryloxy(lower)alkyl, optionally substitutedheterocyclyl(lower)alkyl, optionally substitutedheterocyclyloxy(lower)alkyl, optionally substituted cycloalkyl,optionally substituted cycloalkenyl, optionally substituted aryl oroptionally substituted heterocyclyl and X is optionally substitutedaryl, optionally substituted heterocyclyl, optionally substitutedcycloalkyl or optionally substituted cycloalkenyl.
 22. A method oftreating, preventing or ameliorating a disorder responsive to theblockade of calcium channels in a mammal suffering from said disorder,comprising administering to a mammal in need of such treatment,prevention or amelioration an effective amount of a compound having theFormula I′ described in claim
 19. 23. A method for treating, preventingor ameliorating stroke, neuronal damage resulting from head trauma,epilepsy, pain, migraine, a mood disorder, schizophrenia, aneurodegenerative disorder, depression, anxiety, a psychosis,hypertension or cardiac arrhythmia in a mammal, comprising administeringan effective amount of a compound having the Formula I′ described inclaim
 19. 24. The method of claim 23, wherein the method is fortreating, preventing or ameliorating pain selected from chronic pain,acute pain, and surgical pain.
 25. A method of modulating calciumchannels in a mammal, comprising administering to the mammal at leastone compound having the Formula I′ described in claim
 19. 26. A methodof screening a candidate compound for the ability to bind to a receptorusing a ³H, ¹¹C, or ¹⁴C radiolabeled compound having the Formula I′described in claim 19, comprising a) introducing a fixed concentrationof the radiolabeled compound to the receptor to form a mixture; b)titrating the mixture with a candidate compound; and c) determining thebinding of the candidate compound to said receptor.
 27. Use of acompound having the Formula I′ described in claim 19 in the manufactureof a medicament for the treating, preventing or ameliorating stroke,neuronal damage resulting from head trauma, epilepsy, pain, migraine, amood disorder, schizophrenia, a neurodegenerative disorder, depression,anxiety, a psychosis, hypertension or cardiac arrhythmia in a mammal.28. Use of a compound having the Formula I′ described in claim 19 in themanufacture of a medicament for the treating, preventing or amelioratingpain selected from chronic pain, acute pain, and surgical pain.